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Sample records for surplus plutonium pu

  1. Overview of surplus weapons plutonium disposition

    Energy Technology Data Exchange (ETDEWEB)

    Rudy, G.

    1996-05-01

    The safe disposition of surplus weapons useable plutonium is a very important and urgent task. While the functions of long term storage and disposition directly relate to the Department`s weapons program and the environmental management program, the focus of this effort is particularly national security and nonproliferation.

  2. LLNL MOX fuel lead assemblies data report for the surplus plutonium disposition environmental impact statement

    Energy Technology Data Exchange (ETDEWEB)

    O`Connor, D.G.; Fisher, S.E.; Holdaway, R. [and others

    1998-08-01

    The purpose of this document is to support the US Department of Energy (DOE) Fissile Materials Disposition Program`s preparation of the draft surplus plutonium disposition environmental impact statement. This is one of several responses to data call requests for background information on activities associated with the operation of the lead assembly (LA) mixed-oxide (MOX) fuel fabrication facility. The DOE Office of Fissile Materials Disposition (DOE-MD) has developed a dual-path strategy for disposition of surplus weapons-grade plutonium. One of the paths is to disposition surplus plutonium through irradiation of MOX fuel in commercial nuclear reactors. MOX fuel consists of plutonium and uranium oxides (PuO{sub 2} and UO{sub 2}), typically containing 95% or more UO{sub 2}. DOE-MD requested that the DOE Site Operations Offices nominate DOE sites that meet established minimum requirements that could produce MOX LAs. LLNL has proposed an LA MOX fuel fabrication approach that would be done entirely inside an S and S Category 1 area. This includes receipt and storage of PuO{sub 2} powder, fabrication of MOX fuel pellets, assembly of fuel rods and bundles, and shipping of the packaged fuel to a commercial reactor site. Support activities will take place within a Category 1 area. Building 332 will be used to receive and store the bulk PuO{sub 2} powder, fabricate MOX fuel pellets, and assemble fuel rods. Building 334 will be used to assemble, store, and ship fuel bundles. Only minor modifications would be required of Building 332. Uncontaminated glove boxes would need to be removed, petition walls would need to be removed, and minor modifications to the ventilation system would be required.

  3. Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements.

    Science.gov (United States)

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per

    2014-02-01

    This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation.

  4. Plutonium isotopes 238Pu, 239+240Pu, 241Pu and 240Pu/239Pu atomic ratios in the southern Baltic Sea ecosystem

    Directory of Open Access Journals (Sweden)

    Dagmara I. Strumińska-Parulska

    2010-09-01

    Full Text Available The paper summarizes the results of plutonium findings in atmospheric fallout samples and marine samples from the southern Baltic Sea during our research in 1986-2007. The activities of 238Pu and 239+240Pu isotopes were measured with an alpha spectrometer. The activities of 241Pu were calculated indirectly by 241Am activity measurements 16-18 years after the Chernobyl accident. The 240Pu/239Pu atomic ratios were measured using accelerator mass spectrometry (AMS. The 241Pu activities indicate that the main impact of the Chernobyl accident was on the plutonium concentration in the components of the Baltic Sea ecosystem examined in this work. The highest 241Pu/239+240Pu activity ratio was found in sea water (140 ± 33. The AMS measurements of atmospheric fallout samples collected during 1986 showed a significant increase in the 240Pu/239Pu atomic ratio from 0.29 ± 0.04 in March 1986 to 0.47 ± 0.02 in April 1986.

  5. ANL-W MOX fuel lead assemblies data report for the surplus plutonium disposition environmental impact statement

    Energy Technology Data Exchange (ETDEWEB)

    O`Connor, D.G.; Fisher, S.E.; Holdaway, R. [and others

    1997-08-01

    The purpose of this document is to support the US Department of Energy (DOE) Fissile Materials Disposition Program`s preparation of the draft surplus plutonium disposition environmental impact statement (EIS). This is one of several responses to data call requests for background information on activities associated with the operation of the lead assembly (LA) mixed-oxide (MOX) fuel fabrication facility. The DOE Office of fissile Materials Disposition (DOE-MD) has developed a dual-path strategy for disposition of surplus weapons-grade plutonium. One of the paths is to disposition surplus plutonium through irradiation of MOX fuel in commercial nuclear reactors. MOX fuel consists of plutonium and uranium oxides (PuO{sub 2} and UO{sub 2}), typically containing 95% or more UO{sub 2}. DOE-MD requested that the DOE Site Operations Offices nominate DOE sites that meet established minimum requirements that could produce MOX LAs. The paper describes the following: Site map and the LA facility; process descriptions; resource needs; employment requirements; wastes, emissions, and exposures; accident analysis; transportation; qualitative decontamination and decommissioning; post-irradiation examination; LA fuel bundle fabrication; LA EIS data report assumptions; and LA EIS data report supplement.

  6. LANL MOX fuel lead assemblies data report for the surplus plutonium disposition environmental impact statement

    Energy Technology Data Exchange (ETDEWEB)

    Fisher, S.E.; Holdaway, R.; Ludwig, S.B. [and others

    1998-08-01

    The purpose of this document is to support the US Department of Energy (DOE) Fissile Materials Disposition Program`s preparation of the draft surplus plutonium disposition environmental impact statement. This is one of several responses to data call requests for background information on activities associated with the operation of the lead assembly (LA) mixed-oxide (MOX) fuel fabrication facility. LANL has proposed an LA MOX fuel fabrication approach that would be done entirely inside an S and S Category 1 area. This includes receipt and storage of PuO{sub 2} powder, fabrication of MOX fuel pellets, assembly of fuel rods and bundles, and shipping of the packaged fuel to a commercial reactor site. Support activities will take place within both Category 1 and 2 areas. Technical Area (TA) 55/Plutonium Facility 4 will be used to store the bulk PuO{sub 2} powder, fabricate MOX fuel pellets, assemble rods, and store fuel bundles. Bundles will be assembled at a separate facility, several of which have been identified as suitable for that activity. The Chemistry and Metallurgy Research Building (at TA-3) will be used for analytical chemistry support. Waste operations will be conducted in TA-50 and TA-54. Only very minor modifications will be needed to accommodate the LA program. These modifications consist mostly of minor equipment upgrades. A commercial reactor operator has not been identified for the LA irradiation. Postirradiation examination (PIE) of the irradiated fuel will take place at either Oak Ridge National Laboratory or ANL-W. The only modifications required at either PIE site would be to accommodate full-length irradiated fuel rods. Results from this program are critical to the overall plutonium distribution schedule.

  7. Plutonium stabilization and handling (PuSH)

    Energy Technology Data Exchange (ETDEWEB)

    Weiss, E.V.

    1997-01-23

    This Functional Design Criteria (FDC) addresses construction of a Stabilization and Packaging System (SPS) to oxidize and package for long term storage remaining plutonium-bearing special nuclear materials currently in inventory at the Plutonium Finishing Plant (PFP), and modification of vault equipment to allow storage of resulting packages of stabilized SNM for up to fifty years. The major sections of the project are: site preparation; SPS Procurement, Installation, and Testing; storage vault modification; and characterization equipment additions. The SPS will be procured as part of a Department of Energy nationwide common procurement. Specific design crit1460eria for the SPS have been extracted from that contract and are contained in an appendix to this document.

  8. Migration of plutonium from freshwater ecosystem at Hanford. [/sup 238/Pu, /sup 239/Pu, /sup 240/Pu

    Energy Technology Data Exchange (ETDEWEB)

    Emery, R. M.; Klopfer, D. C.; McShane, M. C.

    1977-09-01

    A reprocessing waste pond at Hanford has been inventoried to determine quantities of plutonium (Pu) that have been accumulated since its formation in 1944. Expressions of export were developed from these inventory data and from informed assumptions about the vectors which act to mobilize material containing Pu. This 14-acre pond provides a realistic illustration of the mobility of Pu in a lentic ecosystem. The ecological behavior of Pu in this pond is similar to that in other contaminated aquatic systems having widely differing limnological characteristics. Since its creation, this pond has received about one Ci of /sup 239/,/sup 240/Pu and /sup 238/Pu, most of which has been retained by its sediments. Submerged plants, mainly diatoms and Potamogeton, accumulate >95% of the Pu contained in biota. Emergent insects are the only direct biological route of export, mobilizing about 5 x 10/sup 3/ nCi of Pu annually, which is also the estimated maximum quantity of the Pu exported by waterfowl, birds and mammals collectively. There is no apparent significant export by wind, and it is not likely that Pu has migrated to the ground water below U-Pond via percolation. Although this pond has a rapid flushing rate, a eutrophic nutrient supply with a diverse biotic profile, and interacts with an active terrestrial environment, it appears to effectively bind Pu and prevent it from entering pathways to man and other life.

  9. 77 FR 44222 - Notice of Availability of the Draft Surplus Plutonium Disposition Supplemental Environmental...

    Science.gov (United States)

    2012-07-27

    ... an oxide form of plutonium suitable for disposition, and the use of mixed oxide (MOX) fuel fabricated... the decision to fabricate 34 metric tons (MT) (37.5 tons) of surplus plutonium into MOX fuel in the MOX Fuel Fabrication Facility (MFFF) (65 FR 1608, January 11, 2000 and 68 FR 20134, April 24,...

  10. Oxidation behaviour of plutonium rich (U, Pu)C and (U, Pu)O2

    Science.gov (United States)

    Sali, S. K.; Kulkarni, N. K.; Phatak, Rohan; Agarwal, Renu

    2016-10-01

    Oxidation behaviour of (U0.3Pu0.7)C1.06 was investigated in air by heating samples up to 1073 K and 1273 K. Thermogravimetry (TG) of the samples and X-ray powder diffraction (XRD) of the intermediate products were used to understand the phenomenon taking place during this process. Theoretical calculations were carried out to understand the multiple phase changes taking place during oxidation of carbide. Theoretical results were validated by XRD analysis of the products obtained at different stages of oxidation. The final oxidized products were found to be a single FCC phase with O/M = 2.15 (M = U + Pu). Oxidation kinetic studies of (U0.3Pu0.7)O2 and (U0.47Pu0.53)O2 were carried out in dry air, using thermogravimetry, under non-isothermal conditions. The activation energy of oxidation was found to be 49 and 70 kJ/mol, respectively. Lattice parameter dependence on Pu/M and O/M of plutonium rich mixed oxide (MOX) was established using combined results of XRD and TG analysis of (U0.3Pu0.7)O2+x and (U0.47Pu0.53)O2+x.

  11. Presence of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, in soils from Chile

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, E., E-mail: echamizo@us.es [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Garcia-Leon, M., E-mail: manugar@us.es [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, Avda. Reina Mercedes sn, 41012 Seville (Spain); Peruchena, J.I., E-mail: jiperuchena@gmail.com [Centro Nacional de Aceleradores, Avda. Thomas Alba Edison, 7, 41092 Sevilla (Spain); Cereceda, F., E-mail: francisco.cereceda@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Vidal, V., E-mail: victor.vidal@usm.cl [Laboratorio de Quimica Ambiental, Centro de Tecnologias Ambientales (CETAM), Universidad Tecnica Federico Santa Maria, Casilla 110-V, Valparaiso (Chile); Pinilla, E., E-mail: epinilla@unex.es [Departamento de Quimica Analitica, Facultad de Ciencias, Universidad de Extremadura, Avda. de Elvas sn, 06071 Badajoz (Spain); Miro, C., E-mail: cmiro@unex.es [Departamento de Fisica Aplicada, Universidad de Extremadura, Avda. de la Universidad sn, 10071 Caceres (Spain)

    2011-12-15

    Plutonium is present in every environmental compartment, due to a variety of nuclear activities. The Southern Hemisphere has received about 20% of the global {sup 239}Pu and {sup 240}Pu environmental inventory, with an important contribution of the so-called tropospheric fallout from both the atmospheric nuclear tests performed in the French Polynesia and in Australia by France and United Kingdom, respectively. In this work we provide new data on the impact of these tests to South America through the study of {sup 239}Pu and {sup 240}Pu in soils from different areas of Northern, Central and Southern Chile. The obtained results point out to the presence of debris from the French tests in the 20-40 Degree-Sign Southern latitude range, with {sup 240}Pu/{sup 239}Pu atomic ratios quite heterogeneous and ranging from 0.02 to 0.23. They are significantly different from the expected one for the global fallout in the Southern Hemisphere for the 30-53 Degree-Sign S latitude range (0.185 {+-} 0.047), but they follow the same trend as the reported values by the Department of Energy of United States for other points with similar latitudes. The {sup 239+240}Pu activity inventories show as well a wider variability range in that latitude range, in agreement with the expected heterogeneity of the contamination.

  12. Supplement to the Surplus Plutonium Disposition Draft Environmental Impact Statement

    Energy Technology Data Exchange (ETDEWEB)

    N/A

    1999-05-14

    On May 22, 1997, DOE published a Notice of Intent in the Federal Register (62 Federal Register 28009) announcing its decision to prepare an environmental impact statement (EIS) that would tier from the analysis and decisions reached in connection with the ''Storage and Disposition of Weapons-Usable Fissile Materials Final Programmatic EIS (Storage and Disposition PEIS)''. ''The Surplus Plutonium Disposition Draft Environmental Impact Statement'' (SPD Draft EIS) (DOWEIS-0283-D) was prepared in accordance with NEPA and issued in July 1998. It identified the potential environmental impacts of reasonable alternatives for the proposed siting, construction, and operation of three facilities for plutonium disposition. These three facilities would accomplish pit disassembly and conversion, immobilization, and MOX fuel fabrication. For the alternatives that included MOX fuel fabrication, the draft also described the potential environmental impacts of using from three to eight commercial nuclear reactors to irradiate MOX fuel. The potential impacts were based on a generic reactor analysis that used actual reactor data and a range of potential site conditions. In May 1998, DCE initiated a procurement process to obtain MOX fuel fabrication and reactor irradiation services. The request for proposals defined limited activities that may be performed prior to issuance of the SPD EIS Record of Decision (ROD) including non-site-specific work associated with the development of the initial design for the MOX fuel fabrication facility, and plans (paper studies) for outreach, long lead-time procurements, regulatory management, facility quality assurance, safeguards, security, fuel qualification, and deactivation. No construction on the proposed MOX facility would begin before an SPD EIS ROD is issued. In March 1999, DOE awarded a contract to Duke Engineering & Services; COGEMA, Inc.; and Stone & Webster (known as DCS) to provide the requested

  13. Determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using radiochemical separation combined with radiometric and mass spectrometric measurements

    DEFF Research Database (Denmark)

    Xu, Yihong; Qiao, Jixin; Hou, Xiaolin

    2014-01-01

    This paper reports an analytical method for the determination of plutonium isotopes (238Pu, 239Pu, 240Pu, 241Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation...

  14. Analysis of plutonium isotope ratios including (238)Pu/(239)Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS.

    Science.gov (United States)

    Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

    2017-04-01

    Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as (238)U with (238)Pu and (241)Am with (241)Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of (238)Pu/(239)Pu, (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the (240)Pu/(239)Pu, (241)Pu/(239)Pu, and (242)Pu/(239)Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, (238)Pu/(239)Pu isotope ratios were able to be calculated by using both the (238)Pu/((239)Pu+(240)Pu) activity ratios that had been measured through alpha spectrometry and the (240)Pu/(239)Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including (238)Pu/(239)Pu, in individual U-Pu mixed oxide particles. Copyright © 2016 Elsevier B.V. All rights reserved.

  15. Hydrolysis of trivalent plutonium and solubility of Pu(OH)3 (am) under electrolytic reducing conditions.

    Science.gov (United States)

    Cho, Hye-Ryun; Youn, Young-Sang; Jung, Euo Chang; Cha, Wansik

    2016-12-06

    The aim of this work is to determine the solubility product of plutonium hydroxide under reducing conditions and to ascertain the stability of Pu(OH)3 (am) in water. Hydrolysis of Pu(iii) and solubility of Pu(OH)3 (am) were investigated at a constant ionic strength of 0.1 M NaClO4. Coulometric titration was adopted to adjust the pH of plutonium solutions, during which the electrolytic reducing conditions maintained the oxidation state of Pu(iii). Chemical speciation for dissolved plutonium was investigated using sensitive spectrophotometry coupled with a liquid waveguide capillary cell. The spectroscopic investigations indicated that dissolved Pu(iv), Pu(v), and Pu(vi) species were ignorable under these experimental conditions. The absorbance of Pu(3+) ions decreased due to hydrolysis of Pu(iii) but the absorbance of Pu(iii) hydrolysis species was not distinguishable. The formation constant for the first hydrolysis species (log (*)β'1) determined in the present study is -6.62 ± 0.25. The non-crystalline structure of the plutonium precipitate was observed through X-ray diffraction. The solubility product of Pu(OH)3 (am), log (*)K's,0 is determined to be 15.23 ± 0.50. These results indicate a stronger tendency for the hydrolysis of Pu(iii) and higher stability (lower solubility) of Pu(OH)3 (am) compared to Am(iii).

  16. 238Pu: accumulation, tissue distribution, and excretion in Mayak workers after exposure to plutonium aerosols.

    Science.gov (United States)

    Suslova, Klara G; Sokolova, Alexandra B; Khokhryakov, Viktor V; Miller, Scott C

    2012-03-01

    The alpha spectrometry measurements of specific activity of 238Pu and 239Pu in urine from bioassay examinations of 1,013 workers employed at the radiochemical and plutonium production facilities of the Mayak Production Association and in autopsy specimens of lung, liver, and skeleton from 85 former nuclear workers who died between 1974-2009, are summarized.The accumulation fraction of 238Pu in the body and excreta has not changed with time in workers involved in production of weapons-grade plutonium production (e.g., the plutonium production facility and the former radiochemical facility). The accumulation fraction of 238Pu in individuals exposed to plutonium isotopes at the newer Spent Nuclear Fuel Reprocessing Plant ranged from 0.13% up to 27.5% based on the autopsy data. No statistically significant differences between 238Pu and 239Pu in distribution by the main organs of plutonium deposition were found in the Mayak workers. Based on the bioassay data,the fraction of 238Pu activity in urine is on average 38-69% of the total activity of 238Pu and 239Pu, which correlates with the isotopic composition in workplace air sampled at the Spent Nuclear Fuel Reprocessing Plant. In view of the higher specific activity of 238Pu, the contribution of 238Pu to the total internal dose, particularly in the skeleton and liver, might be expected to continue to increase, and continued surveillance is recommended.

  17. SRS MOX fuel lead assemblies data report for the surplus plutonium disposition environmental impact statement

    Energy Technology Data Exchange (ETDEWEB)

    O`Connor, D.G.; Fisher, S.E.; Holdaway, R. [and others

    1998-08-01

    The purpose of this document is to support the US Department of Energy (DOE) Fissile Materials Disposition Program`s preparation of the draft surplus plutonium disposition environmental impact statement. This is one of several responses to data call requests for background information on activities associated with the operation of the lead assembly (LA) mixed-oxide (MOX) fuel fabrication facility. DOE-MD requested that the DOE Site Operations Offices nominate DOE sites that meet established minimum requirements that could produce MOX LAs. Six initial site combinations were proposed: (1) Argonne National Laboratory-West (ANL-W) with support from Idaho National Engineering and Environmental Laboratory (INEEL), (2) Hanford, (3) Los Alamos National Laboratory (LANL) with support from Pantex, (4) Lawrence Livermore National Laboratory (LLNL), (5) Oak Ridge Reservation (ORR), and (6) Savannah River Site(SRS). After further analysis by the sites and DOE-MD, five site combinations were established as possible candidates for producing MOX LAs: (1) ANL-W with support from INEEL, (2) Hanford, (3) LANL, (4) LLNL, and (5) SRS. SRS has proposed an LA MOX fuel fabrication approach that would be done entirely inside an S and S Category 1 area. An alternate approach would allow fabrication of fuel pellets and assembly of fuel rods in an S and S Category 2 or 3 facility with storage of bulk PuO{sub 2} and assembly, storage, and shipping of fuel bundles in an S and S Category 1 facility. The total Category 1 approach, which is the recommended option, would be done in the 221-H Canyon Building. A facility that was never in service will be removed from one area, and a hardened wall will be constructed in another area to accommodate execution of the LA fuel fabrication. The non-Category 1 approach would require removal of process equipment in the FB-Line metal production and packaging glove boxes, which requires work in a contamination area. The Immobilization Hot Demonstration Program

  18. Polonium 210Po, uranium (234U, 238U and plutonium (238Pu, 239+240Pu bioaccumulation in marine birds

    Directory of Open Access Journals (Sweden)

    Strumińska-Parulska D. I.

    2013-04-01

    Full Text Available The aim of this work was the determination of 210Po, 234U, 238U, 238Pu and 239+240Pu concentration in marine birds which permanently or temporally live in the southern Baltic Sea coast. We chose 11 species of seabirds: three species permanently residing at southern Baltic Sea, four species of wintering birds and three species of migrating birds. The results show that analyzed radionuclides are non-uniformly distributed in the marine birds. The highest activities of 210Po were observed in feathers, muscles and liver. The highest uranium content was found in liver, rest of viscera and feathers, while plutonium in the digestion organs and feathers. Omnivore seabirds accumulated more polonium, plutonium than species that feed on fish, while herbivore seabirds accumulated more uranium than carnivore.

  19. Site Selection for Surplus Plutonium Disposition Facilities at the Savannah River Site

    Energy Technology Data Exchange (ETDEWEB)

    Wike, L.D.

    2000-08-17

    A site selection study was conducted to evaluate locations for the proposed Surplus Plutonium Disposition Facilities. Facilities to be located include the Mixed Oxide (MOX) Fuel Fabrication Facility, the Pit Disassembly and Conversion Facility (PDCF), and the Plutonium Immobilization Project (PIP) facility. Objectives of the study include: (1) Confirm that the Department of Energy (DOE) selected locations for the MOX and PDCF were suitable based on selected siting criteria, (2) Recommend a site in the vicinity of F Area that is suitable for the PIP, and (3) Identify alternative suitable sites for one or more of these facilities in the event that further geotechnical characterization or other considerations result in disqualification of a currently proposed site.

  20. DOE plutonium disposition study: Pu consumption in ALWRs. Volume 2, Final report

    Energy Technology Data Exchange (ETDEWEB)

    1993-05-15

    The Department of Energy (DOE) has contracted with Asea Brown Boveri-Combustion Engineering (ABB-CE) to provide information on the capability of ABB-CE`s System 80 + Advanced Light Water Reactor (ALWR) to transform, through reactor burnup, 100 metric tonnes (MT) of weapons grade plutonium (Pu) into a form which is not readily useable in weapons. This information is being developed as part of DOE`s Plutonium Disposition Study, initiated by DOE in response to Congressional action. This document Volume 2, provides a discussion of: Plutonium Fuel Cycle; Technology Needs; Regulatory Considerations; Cost and Schedule Estimates; and Deployment Strategy.

  1. Molecular Structure and Bonding in Plutonium Carbides: A Theoretical Study of PuC3.

    Science.gov (United States)

    Molpeceres, Germán; Rayón, Víctor M; Barrientos, Carmen; Largo, Antonio

    2016-04-14

    The most relevant species of plutonium tricarbide were characterized using theoretical methods. The global minimum is predicted to be a fan structure where the plutonium atom is bonded to a quasi-linear C3 unit. A rhombic isomer, shown to be a bicyclic species with transannular C-C bonding, lies about 39 kJ/mol above the fan isomer. A linear PuCCC isomer and a three-membered ring CPuC2 isomer were found to be higher in energy (150 and 195 kJ/mol, respectively, above the predicted global minimum). The possible processes for the formation of these species are discussed, and the IR spectra were predicted to help in possible experimental detection. The nature of the Pu-C interaction has been analyzed in terms of a topological analysis of the electronic density, showing that Pu-C bonding is essentially ionic with a certain degree of covalent character.

  2. DOE Plutonium Disposition Study: Pu consumption in ALWRs. Volume 1, Final report

    Energy Technology Data Exchange (ETDEWEB)

    1993-05-15

    The Department of Energy (DOE) has contracted with Asea Brown Boveri-Combustion Engineering (ABB-CE) to provide information on the capability of ABB-CE`s System 80 + Advanced Light Water Reactor (ALWR) to transform, through reactor burnup, 100 metric tonnes (MT) of weapons grade plutonium (Pu) into a form which is not readily useable in weapons. This information is being developed as part of DOE`s Plutonium Disposition Study, initiated by DOE in response to Congressional action. This document, Volume 1, presents a technical description of the various elements of the System 80 + Standard Plant Design upon which the Plutonium Disposition Study was based. The System 80 + Standard Design is fully developed and directly suited to meeting the mission objectives for plutonium disposal. The bass U0{sub 2} plant design is discussed here.

  3. 77 FR 1920 - Second Amended Notice of Intent To Modify the Scope of the Surplus Plutonium Disposition...

    Science.gov (United States)

    2012-01-12

    ... (MOX) Fuel Fabrication Facility (MFFF), which DOE is constructing at the Savannah River Site (SRS) in... the other alternatives. The MOX fuel alternative is DOE's preferred alternative for surplus plutonium... suitable for MOX fuel fabrication is disposal at the Waste Isolation Pilot Plant (WIPP) in New...

  4. Plutonium {sup 241}Pu in tissues and organs of Cervidae from Northern Poland

    Energy Technology Data Exchange (ETDEWEB)

    Struminska-Parulska, Dagmara I.; Skwarzec, Bogdan [Gdansk Univ. (Poland). Dept. of Environmental Chemistry and Radiochemistry

    2015-07-01

    Livers, kidneys and muscles of large herbivorous animals: roe deer, red deer and fallow deer, collected in Northern Poland, were the subject of the investigation. The concentration of {sup 241}Pu ranged widely between 1.31 ± 0.28 and 214.5 ± 25.8 mBq kg{sup -1} ww and decreased in the order kidney > liver > muscle. The average values of the activity concentrations of {sup 241}Pu were 11.5 ± 1.8 mBq kg{sup -1} ww in muscles, 14.0 ± 2.25 mBq kg{sup -1} ww in liver and 85.5 ± 9.7 mBq kg{sup -1} ww in kidneys. As statistically checked the sampling location, sex, age and species of animals did not influence on plutonium concentrations of the analyzed samples. Only the organ type significantly influenced {sup 241}Pu content. The values of {sup 241}Pu/{sup 29+240}Pu activity ratio in analyzed samples ranged from 7.12 ± 2.15 to 99.3 ± 16.4 and the results showed the main source of plutonium in analyzed organs could be the Chernobyl accident.

  5. Critical experiments with mixed plutonium-uranium nitrate solutions having Pu:(Pu + U) ratios greater than 0.5

    Energy Technology Data Exchange (ETDEWEB)

    Primm, R.T. III [Oak Ridge National Lab., TN (United States); Lloyd, R.C.; Clayton, E.D. [Pacific Northwest Lab., Richland, WA (United States)

    1986-04-01

    A series of critical experiments was conducted with mixed plutonium-uranium nitrate solutions having Pu:(Pu+U) ratios >0.5. Three geometries and four conditions of reflection were examined. The plutonium concentrations ranged from 170 to 350 g/L. The value of k-effective for each experiment was calculated using the KENO-IV code and 27-group cross sections derived from the Evaluated Nuclear Data File B--version IV (ENDF/B-IV). The mean value for the set of 26 experiments was 1.003, with a minimum value of 0.987 and a maximum of 1.022. The spread in the distribution of calculated k-effectives is believed to be the result of uncertainties in analytical chemistry measurements. No correlation between condition of reflection and calculated k-effective was found. An allowable multiplication factor to be used in the evaluation of reprocessing equipment at conditions that have been investigated was calculated to be 0.945.

  6. Direct isotope ratio analysis of individual uranium-plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry.

    Science.gov (United States)

    Suzuki, Daisuke; Esaka, Fumitaka; Miyamoto, Yutaka; Magara, Masaaki

    2015-02-01

    Uranium and plutonium isotope ratios in individual uranium-plutonium (U-Pu) mixed particles with various U/Pu atomic ratios were analyzed without prior chemical separation by thermal ionization mass spectrometry (TIMS). Prior to measurement, micron-sized particles with U/Pu ratios of 1, 5, 10, 18, and 70 were produced from uranium and plutonium certified reference materials. In the TIMS analysis, the peaks of americium, plutonium, and uranium ion signals were successfully separated by continuously increasing the evaporation filament current. Consequently, the uranium and plutonium isotope ratios, except the (238)Pu/(239)Pu ratio, were successfully determined for the particles at all U/Pu ratios. This indicates that TIMS direct analysis allows for the measurement of individual U-Pu mixed particles without prior chemical separation.

  7. Surplus weapons-grade plutonium: a resource for exploring and terraforming Mars

    Energy Technology Data Exchange (ETDEWEB)

    Muscatello, A.C.; Houts, M.G.

    1996-12-31

    With the end of the Cold War, greater than 100 metric tons (MT) of weapons-grade plutonium (WGPu) have become surplus to defense needs in the United States and the Former Soviet Union. This paper is a proposal for an option for WGPu disposition, i.e., use of the plutonium as a fuel for nuclear reactors for Mars exploration and eventual terraforming. WGPu was used in nuclear weapons because it has a much smaller critical mass than highly enriched uranium, allowing lighter weapons with consequent longer ranges. Similarly, WGPu reactors would also require smaller amounts of fuel to attain a critical mass, making the reactor much lighter overall and resulting in large savings in launch costs. The greater than 100 MT of WGPu would generate about 1000 billion kilowatt hours of heat energy, much of which could be converted into electricity. The waste heat would also be useful to a Martian outpost or colony. A potential way of getting the WGPu reactors into space is a large gas gun like that being developed at the Lawrence Livermore National Laboratory to orbit materials by achieving high velocity at the surface, greatly reducing launch costs and enhancing reliability. Reactor components would be launched on conventional rockets or space shuttles, the reactor fuel rods would be injected into orbit using the gas gun, and the reactor would be assembled in space. Implementation of this proposal would allow disposition of a serious, expensive problem on earth by removing the WGPu from the planet and simultaneously provide a very large energy resource for Mars exploration and terraforming.

  8. Evaluation of alternatives for the disposition of surplus weapons-usable plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Dyer, J.S.; Butler, J.C. [Univ. of Texas, Austin, TX (United States); Edmunds, T. [Lawrence Livermore National Lab., CA (United States)] [and others

    1997-04-04

    The Department of Energy Record of Decision (ROD) selected alternatives for disposition of surplus, weapons grade plutonium. A major objective of this decision was to prevent the proliferation of nuclear weapons. Other concerns addressed included economic, technical, institutional, schedule, environmental, and health and safety issues. The analysis reported here was conducted in parallel with technical, environmental, and nonproliferation analyses; it uses multiattribute utility theory to combine these considerations in order to facilitate an integrated evaluation of alternatives. This analysis is intended to provide additional insight regarding alternative evaluation and to assist in understanding the rationale for the choice of alternatives recommended in the ROD. Value functions were developed for objectives of disposition, and used to rank alternatives. Sensitivity analyses indicated that the ranking of alternatives for the base case was relatively insensitive to changes in assumptions over reasonable ranges. The analyses support the recommendation of the ROD to pursue parallel development of the vitrification immobilization alternative and the use of existing light water reactors alternative. 27 refs., 109 figs., 20 tabs.

  9. Hanford MOX fuel lead assemblies data report for the surplus plutonium disposition environmental impact statement

    Energy Technology Data Exchange (ETDEWEB)

    O`Connor, D.G.; Fisher, S.E.; Holdaway, R. [and others

    1998-08-01

    The purpose of this document is to support the US Department of Energy (DOE) Fissile Materials Disposition Program`s preparation of the draft surplus plutonium disposition environmental impact statement. This is one of several responses to data call requests for background information on activities associated with the operation of the lead assembly (LA) mixed-oxide (MOX) fuel fabrication facility. DOE-MD requested that the DOE Site Operations Offices nominate DOE sites that meet established minimum requirements that could produce MOX LAs. Six initial site combinations were proposed: (1) Argonne National Laboratory-West (ANL-W) with support from Idaho National Engineering and Environmental Laboratory (INEEL), (2) Hanford, (3) Los Alamos National Laboratory (LANL) with support from Pantex, (4) Lawrence Livermore National Laboratory (LLNL), (5) Oak Ridge Reservation (ORR), and (6) Savannah River Site (SRS). After further analysis by the sites and DOE-MD, five site combinations were established as possible candidates for producing MOX LAs: (1) ANL-W with support from INEEL, (2) Hanford, (3) LANL, (4) LLNL, and (5) SRS. Hanford has proposed an LA MOX fuel fabrication approach that would be done entirely inside an S and S Category 1 area. An alternate approach would allow fabrication of fuel pellets and assembly of fuel rods in an S and S Category 1 facility. In all, a total of three LA MOX fuel fabrication options were identified by Hanford that could accommodate the program. In every case, only minor modification would be required to ready any of the facilities to accept the equipment necessary to accomplish the LA program.

  10. Plutonium concentration and (240)Pu/(239)Pu atom ratio in biota collected from Amchitka Island, Alaska: recent measurements using ICP-SFMS.

    Science.gov (United States)

    Bu, Kaixuan; Cizdziel, James V; Dasher, Douglas

    2013-10-01

    Three underground nuclear tests, including the Unites States' largest, were conducted on Amchitka Island, Alaska. Monitoring of the radiological environment around the island is challenging because of its remote location. In 2008, the Department of Energy (DOE) Office of Legacy Management (LM) became responsible for the long term maintenance and surveillance of the Amchitka site. The first DOE LM environmental survey occurred in 2011 and is part of a cycle of activities that will occur every 5 years. The University of Alaska Fairbanks, a participant in the 2011 study, provided the lichen (Cladonia spp.), freshwater moss (Fontinalis neomexicanus), kelp (Eualaria fistulosa) and horse mussel (Modiolus modiolus) samples from Amchitka Island and Adak Island (a control site). These samples were analyzed for (239)Pu and (240)Pu concentration and (240)Pu/(239)Pu atom ratio using inductively coupled plasma sector field mass spectrometry (ICP-SFMS). Plutonium concentrations and (240)Pu/(239)Pu atom ratios were generally consistent with previous terrestrial and marine studies in the region. The ((239)+)(240)Pu levels (mBq kg(-1), dry weight) ranged from 3.79 to 57.1 for lichen, 167-700 for kelp, 27.9-148 for horse mussel, and 560-573 for moss. Lichen from Adak Island had higher Pu concentrations than Amchitka Island, the difference was likely the result of the higher precipitation at Adak compared to Amchitka. The (240)Pu/(239)Pu atom ratios were significantly higher in marine samples compared to terrestrial and freshwater samples (t-test, p Pu occurred into the North Pacific Ocean, likely from the Marshall Island high yield nuclear tests, but other potential sources, such as the Kamchatka Peninsula Rybachiy Naval Base and Amchitka Island underground nuclear test site cannot be ruled out.

  11. Characterization of Representative Materials in Support of Safe, Long Term Storage of Surplus Plutonium in DOE-STD-3013 Containers

    Energy Technology Data Exchange (ETDEWEB)

    Narlesky, Joshua E. [Los Alamos National Laboratory; Stroud, Mary Ann [Los Alamos National Laboratory; Smith, Paul Herrick [Los Alamos National Laboratory; Wayne, David M. [Los Alamos National Laboratory; Mason, Richard E. [MET-1: ACTINIDE PROCESSING SUPPORT; Worl, Laura A. [Los Alamos National Laboratory

    2013-02-15

    The Surveillance and Monitoring Program is a joint Los Alamos National Laboratory/Savannah River Site effort funded by the Department of Energy-Environmental Management to provide the technical basis for the safe, long-term storage (up to 50 years) of over 6 metric tons of plutonium stored in over 5,000 DOE-STD-3013 containers at various facilities around the DOE complex. The majority of this material is plutonium that is surplus to the nuclear weapons program, and much of it is destined for conversion to mixed oxide fuel for use in US nuclear power plants. The form of the plutonium ranges from relatively pure metal and oxide to very impure oxide. The performance of the 3013 containers has been shown to depend on moisture content and on the levels, types and chemical forms of the impurities. The oxide materials that present the greatest challenge to the storage container are those that contain chloride salts. Other common impurities include oxides and other compounds of calcium, magnesium, iron, and nickel. Over the past 15 years the program has collected a large body of experimental data on 54 samples of plutonium, with 53 chosen to represent the broader population of materials in storage. This paper summarizes the characterization data, moisture analysis, particle size, surface area, density, wattage, actinide composition, trace element impurity analysis, and shelf life surveillance data and includes origin and process history information. Limited characterization data on fourteen nonrepresentative samples is also presented.

  12. Observed changes in the mechanism and rates of Pu(V) reduction on hematite as a function of total plutonium concentration.

    Science.gov (United States)

    Hixon, Amy E; Powell, Brian A

    2014-08-19

    Changes in aqueous- and solid-phase plutonium oxidation states were monitored as a function of time and plutonium concentration in hematite (α-Fe2O3) suspensions containing initially Pu(V). Batch kinetic experiments were conducted at plutonium concentrations between 10(-8) and 10(-6) M at pH 5 and 0.3 g/L (9.3 m(2)/L) hematite. Surface-mediated reduction of Pu(V) was observed under all conditions studied. However, differences in the reaction kinetics demonstrate that the mechanism of Pu(V) reduction changes as a function of plutonium concentration. Adsorption of Pu(V) was found to be the rate-limiting step at plutonium concentrations less than approximately 10(-7) M Pu(V). Plutonium reduction in these systems was attributed to trace amounts of Fe(II) in the hematite structure. Reduction of Pu(V) was found to be the rate-limiting step at concentrations higher than approximately 10(-6) M Pu(V) and is attributed to the formation of PuO(2+x)·nH2O nanoparticles and the Nernstian favorability of Pu(IV) surface complexes. The reaction order with respect to plutonium concentration was found to be -0.68 ± 0.09, indicating that there is a concentration dependence in these systems. This work strongly suggests that the kinetics of experiments carried out under high plutonium concentrations (i.e., >10(-7) M Pu) cannot be directly extrapolated to environmental concentrations of plutonium.

  13. LLNL Site plan for a MOX fuel lead assembly mission in support of surplus plutonium disposition

    Energy Technology Data Exchange (ETDEWEB)

    Bronson, M.C.

    1997-10-01

    The principal facilities that LLNL would use to support a MOX Fuel Lead Assembly Mission are Building 332 and Building 334. Both of these buildings are within the security boundary known as the LLNL Superblock. Building 332 is the LLNL Plutonium Facility. As an operational plutonium facility, it has all the infrastructure and support services required for plutonium operations. The LLNL Plutonium Facility routinely handles kilogram quantities of plutonium and uranium. Currently, the building is limited to a plutonium inventory of 700 kilograms and a uranium inventory of 300 kilograms. Process rooms (excluding the vaults) are limited to an inventory of 20 kilograms per room. Ongoing operations include: receiving SSTS, material receipt, storage, metal machining and casting, welding, metal-to-oxide conversion, purification, molten salt operations, chlorination, oxide calcination, cold pressing and sintering, vitrification, encapsulation, chemical analysis, metallography and microprobe analysis, waste material processing, material accountability measurements, packaging, and material shipping. Building 334 is the Hardened Engineering Test Building. This building supports environmental and radiation measurements on encapsulated plutonium and uranium components. Other existing facilities that would be used to support a MOX Fuel Lead Assembly Mission include Building 335 for hardware receiving and storage and TRU and LLW waste storage and shipping facilities, and Building 331 or Building 241 for storage of depleted uranium.

  14. On the multi-reference nature of plutonium oxides: PuO2(2+), PuO2, PuO3 and PuO2(OH)2.

    Science.gov (United States)

    Boguslawski, Katharina; Réal, Florent; Tecmer, Paweł; Duperrouzel, Corinne; Gomes, André Severo Pereira; Legeza, Örs; Ayers, Paul W; Vallet, Valérie

    2017-02-08

    Actinide-containing complexes present formidable challenges for electronic structure methods due to the large number of degenerate or quasi-degenerate electronic states arising from partially occupied 5f and 6d shells. Conventional multi-reference methods can treat active spaces that are often at the upper limit of what is required for a proper treatment of species with complex electronic structures, leaving no room for verifying their suitability. In this work we address the issue of properly defining the active spaces in such calculations, and introduce a protocol to determine optimal active spaces based on the use of the Density Matrix Renormalization Group algorithm and concepts of quantum information theory. We apply the protocol to elucidate the electronic structure and bonding mechanism of volatile plutonium oxides (PuO3 and PuO2(OH)2), species associated with nuclear safety issues for which little is known about the electronic structure and energetics. We show how, within a scalar relativistic framework, orbital-pair correlations can be used to guide the definition of optimal active spaces which provide an accurate description of static/non-dynamic electron correlation, as well as to analyse the chemical bonding beyond a simple orbital model. From this bonding analysis we are able to show that the addition of oxo- or hydroxo-groups to the plutonium dioxide species considerably changes the π-bonding mechanism with respect to the bare triatomics, resulting in bent structures with a considerable multi-reference character.

  15. Plutonium Isotopes ((239-241)Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed.

    Science.gov (United States)

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Golser, Robin; Gómez-Guzmán, José Manuel; Korschinek, Gunther; Kortmann, Florian; Lierse von Gostomski, Christoph; Ludwig, Peter; Steier, Peter; Tazoe, Hirofumi; Yamada, Masatoshi

    2017-02-21

    The concentration of plutonium (Pu) and the isotopic ratios of (240)Pu to (239)Pu and (241)Pu to (239)Pu were determined by accelerator mass spectrometry (AMS) in Pacific Ocean water samples (20 L each) collected in late 2012. The isotopic Pu ratios are important indicators of different contamination sources and were used to identify a possible release of Pu into the ocean by the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. In particular, (241)Pu is a well-suited indicator for a recent entry of Pu because (241)Pu from fallout of nuclear weapon testings has already significantly decayed. A total of 10 ocean water samples were prepared at the Radiochemie München of the TUM and analyzed at the Vienna Environmental Research Laboratory (VERA). Several samples showed a slightly elevated (240)Pu/(239)Pu ratio of up to 0.22 ± 0.02 compared to global fallout ((240)Pu/(239)Pu = 0.180 ± 0.007), whereas all measured (241)Pu-to-(239)Pu ratios were consistent with nuclear weapon fallout ((241)Pu/(239)Pu < 2.4 × 10(-3)), which means that no impact from the Fukushima accident was detected. From the average (241)Pu-to-(239)Pu ratio of 8-2(+3) ×10(-4) at a sampling station located at a distance of 39.6 km to FDNPP, the 1-σ upper limit for the FDNPP contribution to the (239)Pu inventory in the water column was estimated to be 0.2%. Pu, with the signature of weapon-grade Pu was found in a single sample collected around 770 km off the west coast of the United States.

  16. An ab initio study of plutonium oxides surfaces; Etude ab initio des surfaces d'oxydes de Pu

    Energy Technology Data Exchange (ETDEWEB)

    Jomard, G.; Bottin, F.; Amadon, B

    2007-07-01

    By means of first-principles calculations, we have studied the atomic structure as well as the thermodynamic stability of various plutonium dioxide surfaces in function of their environment (in terms of oxygen partial pressure and temperature). All these simulations have been performed with the ABINIT code. It is well known that DFT fails to describe correctly plutonium-based materials since 5f electrons in such systems are strongly correlated. In order to go beyond DFT, we have treated PuO{sub 2} and {beta}-Pu{sub 2}O{sub 3} in a DFT+U framework. We show that the couple of parameters (U,J) that works well for pure Pu is also well designed for describing ground state (GS) properties of these two oxides. The major improvement with respect with DFT is that we are able to predict an insulating GS in agreement with experiments. The presence of a gap in the DOS (Density of States) of plutonium oxides should play a significant role in the predicted surface reactivity. However, performing DFT+U calculations on surfaces of plutonium oxide from scratch was too ambitious. That is why we decided, as a first step, to study the stability of the (100), (110) and (111) surfaces of PuO{sub 2} in a DFT-GGA framework. For each of these orientations, we considered various terminations. These ab initio results have been introduced in a thermodynamic model which allows us to predict the relative stability of the different terminations as a function of temperature and oxygen partial pressure (p{sub O{sub 2}}). We conclude that at room temperature and for p{sub O{sub 2}}{approx}10 atm., the polar O{sub 2}-(100) termination is favoured. The stabilization of such a polar stoichiometric surface is surprising and should be confirmed by DFT+U calculations before any final conclusion. (authors)

  17. Disposition of transuranic residues from plutonium isentropic compression experiment (Pu-ice) conducted at Z machine

    Energy Technology Data Exchange (ETDEWEB)

    Goyal, Kapil K [Los Alamos National Laboratory; French, David M [Los Alamos National Laboratory; Humphrey, Betty J [WESTON SOLUTIONS INC.; Gluth, Jeffry [SNL

    2010-01-01

    In 1992, the U.S. Congress passed legislation to discontinue above- and below-ground testing of nuclear weapons. Because of this, the U.S. Department of Energy (DOE) must rely on laboratory experiments and computer-based calculations to verify the reliability of the nation's nuclear stockpile. The Sandia National Laboratories/New Mexico (SNL/NM) Z machine was developed by the DOE to support its science-based approach to stockpile stewardship. SNL/NM researchers also use the Z machine to test radiation effects on various materials in experiments designed to mimic nuclear explosions. Numerous components, parts, and materials have been tested. These experiments use a variety of radionuclides; however, plutonium (Pu) isotopes with greater than ninety-eight percent enrichment are the primary radionuclides used in the experiments designed for stockpile stewardship. In May 2006, SNL/NM received authority that the Z Machine Isentropic Compression Experiments could commence. Los Alamos National Laboratory (LANL) provided the plutonium targets and loaded the target assemblies, which were fabricated by SNL/NM. LANL shipped the loaded assemblies to SNL/NM for Z machine experiments. Three experiments were conducted from May through July 2006. The residues from each experiment, which weighed up to 913 pounds, were metallic and packaged into a respective 55-gallon drum each. Based on a memorandum of understanding between the two laboratories, LANL provides the plutonium samples and the respective radio-isotopic information. SNL/NM conducts the experiments and provides temporary storage for the drums until shipment to LANL for final waste certification for disposal at the Waste Isolation Pilot Plant (WIPP) in southeastern New Mexico. This paper presents a comprehensive approach for documenting generator knowledge for characterization of waste in cooperation with scientists at the two laboratories and addresses a variety of topics such as material control and accountability

  18. Oxidation states, geometries, and electronic structures of plutonium tetroxide PuO4 isomers: is octavalent Pu viable?

    Science.gov (United States)

    Huang, Wei; Xu, Wen-Hua; Su, Jing; Schwarz, W H E; Li, Jun

    2013-12-16

    In neutral chemical compounds, the highest known oxidation state of all elements in the Periodic Table is +VIII. While PuO4 is viewed as an exotic Pu(+VIII) complex, we have shown here that no stable electronic homologue of octavalent RuO4 and OsO4 exists for PuO4, even though Pu has the same number of eight valence electrons as Ru and Os. Using quantum chemical approaches at the levels of quasi-relativistic DFT, MP2, CCSD(T), and CASPT2, we find the ground state of PuO4 as a quintet (5)C2v-(PuO2)(+)(O2)(-) complex with the leading valence configuration of an (f(3))plutonyl(V) unit, loosely coupled to a superoxido (π*(3))O2(-) ligand. This stable isomer is likely detectable as a transient species, while the previously suggested planar (1)D4h-Pu(VIII)O4 isomer is only metastable. Through electronic structure analyses, the bonding and the oxidation states are explained and rationalized. We have predicted the characteristics of the electronic and vibrational spectra to assist future experimental identification of (PuO2)(+)(O2)(-) by IR, UV-vis, and ionization spectroscopy.

  19. DFT and two-dimensional correlation analysis methods for evaluating the Pu{sup 3+}–Pu{sup 4+} electronic transition of plutonium-doped zircon

    Energy Technology Data Exchange (ETDEWEB)

    Bian, Liang, E-mail: bianliang@ms.xjb.ac.cn [Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, Xinjiang (China); Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China); Dong, Fa-qin; Song, Mian-xin [Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China); Dong, Hai-liang [Department of Geology and Environmental Earth Science, Miami University, Oxford, OH 45056 (United States); Li, Wei-Min [Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, Xinjiang (China); Duan, Tao; Xu, Jin-bao [Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China); Zhang, Xiao-yan [Key Laboratory of Functional Materials and Devices for Special Environments, Chinese Academy of Sciences, Urumqi 830011, Xinjiang (China); Laboratory for Extreme Conditions Matter Properties, South West University of Science and Technology, Mianyang 621010, Sichuan (China)

    2015-08-30

    Highlights: • Effect of Pu f-shell electron on the electronic property of zircon is calculated via DFT and 2D-CA techniques. • Reasons of Pu f-shell electron influencing on electronic properties are systematically discussed. • Phase transitions are found at two point 2.8 mol% and 7.5 mol%. - Abstract: Understanding how plutonium (Pu) doping affects the crystalline zircon structure is very important for risk management. However, so far, there have been only a very limited number of reports of the quantitative simulation of the effects of the Pu charge and concentration on the phase transition. In this study, we used density functional theory (DFT), virtual crystal approximation (VCA), and two-dimensional correlation analysis (2D-CA) techniques to calculate the origins of the structural and electronic transitions of Zr{sub 1−c}Pu{sub c}SiO{sub 4} over a wide range of Pu doping concentrations (c = 0–10 mol%). The calculations indicated that the low-angular-momentum Pu-f{sub xy}-shell electron excites an inner-shell O-2s{sup 2} orbital to create an oxygen defect (V{sub O-s}) below c = 2.8 mol%. This oxygen defect then captures a low-angular-momentum Zr-5p{sup 6}5s{sup 2} electron to form an sp hybrid orbital, which exhibits a stable phase structure. When c > 2.8 mol%, each accumulated V{sub O-p} defect captures a high-angular-momentum Zr-4d{sub z} electron and two Si-p{sub z} electrons to create delocalized Si{sup 4+} → Si{sup 2+} charge disproportionation. Therefore, we suggest that the optimal amount of Pu cannot exceed 7.5 mol% because of the formation of a mixture of ZrO{sub 8} polyhedral and SiO{sub 4} tetrahedral phases with the orientation (10-1). This study offers new perspective on the development of highly stable zircon-based solid solution materials.

  20. On the Multi-Reference Nature of Plutonium Oxides: PuO$_2^{2+}$, PuO$_2$, PuO$_3$ and PuO$_2$(OH)$_2$

    CERN Document Server

    Boguslawski, Katharina; Tecmer, Paweł; Duperrouzel, Corinne; Gomes, André Severo Pereira; Legeza, Örs; Ayers, Paul W; Vallet, Valérie

    2016-01-01

    Actinide-containing complexes present formidable challenges for electronic structure methods due to the large number of degenerate or quasi-degenerate electronic states arising from partially occupied 5f and 6d shells. Conventional multi-reference methods can treat active spaces that are often at the upper limit of what is required for a proper treatment of species with complex electronic structures, leaving no room for verifying their suitability. In this work we address the issue of properly defining the active spaces in such calculations, and introduce a protocol to determine optimal active spaces based on the use of the Density Matrix Renormalization Group algorithm and concepts of quantum information theory. We apply the protocol to elucidate the electronic structure and bonding mechanism of volatile plutonium oxides (PuO$_3$ and PuO$_2$(OH)$_2$), species associated with nuclear safety issues for which little is known about the electronic structure and energetics. We show how, within a scalar relativisti...

  1. Resolving Nevada Test Site and global fallout plutonium in attic dust and soils using [sup 137]Cs/[sup 239+240]Pu activity ratios

    Energy Technology Data Exchange (ETDEWEB)

    Cizdziel, J. (Univ. of Nevada, Reno, NV (United States)); Hodge, V. (Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry); Faller, S. (Environmental Protection Agency, Las Vegas, NV (United States). Radiation and Indoor Environments National Lab.)

    1999-07-01

    A simple equation using only [sup 137]Cs/[sup 239+240]Pu activity ratios was developed and evaluated as a means of resolving the plutonium in attic dust and soil from Nevada and Utah that came from Nevada Test Site fallout from that which came from global fallout. Applied to a historical data set of [sup 137]Cs and [sup 239+240]Pu activity concentrations in soils from Nevada and Utah, the activity ratio method gives results similar to the traditional [sup 240]Pu/[sup 239]Pu isotope mass ratio method. Considering the difficulty and expense of determining the [sup 240]Pu/[sup 239]Pu atom ratios, this activity ratio method is simpler, faster, and less costly, and may be useful for detecting and/or monitoring plutonium contamination in soils. Applied to samples of attic dust and soil collected from throughout southern Nevada and Utah during 1996 and 1997, it was found that all sites surveyed showed the presence of Nevada Test Site plutonium. Over 90% of the plutonium found in the samples from Beatty, Tonopah, and Queen City Summit, Nevada can be attributed to the Nevada Test Site.

  2. Study of the Effect of (U0.8Pu0.2O2 Uranium–Plutonium Mixed Fuel Fission Products on a Living Organism

    Directory of Open Access Journals (Sweden)

    Ayagoz Baimukhanova

    2016-08-01

    Full Text Available The article describes the results of experiments conducted on pigs to determine the effect of plutonium, which is the most radiotoxic and highly active element in the range of mixed fuel (U0.8Pu0.2O2 fission products, on living organisms. The results will allow empirical prediction of the emergency plutonium radiation dose for various organs and tissues of humans in case of an accident in a reactor running on mixed fuel (U0.8Pu0.2O2.

  3. Microdistribution and Long-Term Retention of 239Pu (NO3)4 in the Respiratory Tracts of an Acutely Exposed Plutonium Worker and Experimental Beagle Dogs

    Energy Technology Data Exchange (ETDEWEB)

    Nielsen, Christopher E.; Wilson, Dulaney A.; Brooks, Antone L.; McCord, Stacey; Dagle, Gerald E.; James, Anthony C.; Tolmachev, Sergei Y.; Thrall, Brian D.; Morgan, William F.

    2012-11-01

    The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [239Pu (NO3)4] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histological lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a non-uniform distribution of plutonium throughout the lung tissue. Fibrotic scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the sub-pleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential increase in cancer risk.

  4. Microdistribution and long-term retention of 239Pu (NO3)4 in the respiratory tracts of an acutely exposed plutonium worker and experimental beagle dogs.

    Science.gov (United States)

    Nielsen, Christopher E; Wilson, Dulaney A; Brooks, Antone L; McCord, Stacey L; Dagle, Gerald E; James, Anthony C; Tolmachev, Sergei Y; Thrall, Brian D; Morgan, William F

    2012-11-01

    The long-term retention of inhaled soluble forms of plutonium raises concerns as to the potential health effects in persons working in nuclear energy or the nuclear weapons program. The distributions of long-term retained inhaled plutonium-nitrate [(239)Pu (NO(3))(4)] deposited in the lungs of an accidentally exposed nuclear worker (Human Case 0269) and in the lungs of experimentally exposed beagle dogs with varying initial lung depositions were determined via autoradiographs of selected histologic lung, lymph node, trachea, and nasal turbinate tissue sections. These studies showed that both the human and dogs had a nonuniform distribution of plutonium throughout the lung tissue. Fibrotic scar tissue effectively encapsulated a portion of the plutonium and prevented its clearance from the body or translocation to other tissues and diminished dose to organ parenchyma. Alpha radiation activity from deposited plutonium in Human Case 0269 was observed primarily along the subpleural regions while no alpha activity was seen in the tracheobronchial lymph nodes of this individual. However, relatively high activity levels in the tracheobronchial lymph nodes of the beagles indicated the lymphatic system was effective in clearing deposited plutonium from the lung tissues. In both the human case and beagle dogs, the appearance of retained plutonium within the respiratory tract was inconsistent with current biokinetic models of clearance for soluble forms of plutonium. Bound plutonium can have a marked effect on the dose to the lungs and subsequent radiation exposure has the potential to increase cancer risk.

  5. Reactivity of the uranium (U(IV)/U(VI)) and the plutonium (Pu(III)/Pu(IV)) in nitric aqueous solution under ultrasound; De l'influence des ultrasons sur la reactivite de l'uranium (U(IV)/U(VI)) et du plutonium (PU(III)/PU(IV)) en solution aqueuse nitrique

    Energy Technology Data Exchange (ETDEWEB)

    Venault, L

    1998-07-01

    To minimize the volumes of solid waste and industrial effluents generated at the end of cycle, particularly in the spent nuclear fuel reprocessing industry, research is currently under way on so-called innovative processes, designed to induce chemical reactions without adding reagent to the media. Among these processes, the use of ultrasound can prove advantageous, and the purpose of this study is to assess accurately the potential for its application. In the present context, this work shows that the transmission of an ultrasonic wave in aqueous nitric acid solution leads to: the accumulation of nitrous acid in solution, until a steady-sate concentration is reached; the removal of nitrogen monoxide and nitrogen dioxide in the gas stream. The initial kinetics of the formation of HNO{sub 2} in solution was quantified as a function of the nitric acid concentration and the ultrasound intensity. It was also shown than an excess of nitrous acid in nitric solution decomposes under the effect of ultrasound. It is also possible to accumulate hydrogen peroxide in solution during the ultrasonic irradiation of aqueous nitric acid solutions in the presence of a chemical species (N{sub 2}H{sub 5}{sup +}, NH{sub 2}SO{sub 3}H...) which reacts rapidly with HNO{sub 2}, preventing the reduction of H{sub 2}O{sub 2} by HNO{sub 2}. The mechanisms of HNO{sub 2} formation and decomposition, and the mechanism of H{sub 2}O{sub 2} formation during the ultrasonic irradiation of aqueous nitric acid solutions, are presented. Control of H{sub 2}O{sub 2} or HNO{sub 2} in a nitric acid medium under the effect of an ultrasonic wave can be exploited to control redox reactions of uranium and plutonium ions, particularly with respect to the oxidation of U and Pu (U(IV){yields} U(IV) or Pu(III) {yields} Pu(IV)) and the reduction of Pu (Pu(IV){yields} Pu(III). The redox behavior of uranium and plutonium ions in aqueous nitric solution subject to an ultrasonic flux is interpreted in term of effects

  6. Simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu by high resolution inductively coupled plasma mass spectrometer (HR ICP-MS) in marine sediments; Mesure des isotopes du plutonium des sediments marins par spectrometrie de masse a plasma couple inductivement haute resolution (HR ICP-MS)

    Energy Technology Data Exchange (ETDEWEB)

    Bruneau, F

    1999-07-01

    Transuranics elements are of particular interest in radioecological studies because of their radiotoxicity and their potential use to decipher source fingerprints and transport processes. The simultaneous measurement of {sup 239}Pu, {sup 240}Pu, {sup 241}Pu, and {sup 242}Pu in environmental samples requires a specific chemical procedure. This work deals with an analytical procedure which yields a very high grade of purification of Pu suitable for ultra low level detection by HR ICP-MS, from marine sediments. After the elimination of major elements (Fe, Al, Mg...) by a first chromatographic separation, a new device of purification by solvent extraction and concentration by a second chromatographic separation is used to obtain a concentrated and high purified solution of plutonium. The chemical procedure have been validated on IAEA certified sediment samples and on sediment samples collected in the roads of Cherbourg which had been previously analysed by other techniques (a spectrometry and thermo-ionisation mass spectrometer). (author)

  7. Three-component U-Pu-Th fuel for plutonium irradiation in heavy water reactors

    Directory of Open Access Journals (Sweden)

    Peel Ross

    2016-01-01

    Full Text Available This paper discusses concepts for three-component fuel bundles containing plutonium, uranium and thorium for use in pressurised heavy water reactors, and cases for and against implementation of such a nuclear energy system in the United Kingdom. Heavy water reactors are used extensively in Canada, and are deploying within India and China, whilst the UK is considering the use of heavy water reactors to manage its plutonium inventory of 140 tonnes. The UK heavy water reactor proposal uses a mixed oxide (MOX fuel of plutonium in depleted uranium, within the enhanced CANDU-6 (EC-6 reactor. This work proposes an alternative heterogeneous fuel concept based on the same reactor and CANFLEX fuel bundle, with eight large-diameter fuel elements loaded with natural thorium oxide and 35 small-diameter fuel elements loaded with a MOX of plutonium and reprocessed uranium stocks from UK MAGNOX and AGR reactors. Indicative neutronic calculations suggest that such a fuel would be neutronically feasible. A similar MOX may alternatively be fabricated from reprocessed <5% enriched light water reactor fuel, such as the fuel of the AREVA EPR reactor, to consume newly produced plutonium from reprocessing, similar to the DUPIC (direct use of PWR fuel in CANDU process.

  8. Determination of Pu-238 Abundance in a Plutonium Standard by an Advanced Thermal Ionization Mass Spectrometric Technique

    Science.gov (United States)

    Mason, P.; Thomas, R.

    2006-12-01

    New developments in thermal ionization mass spectrometers allow for the determination of very small minor isotope ratios. The new hardware and software capabilities require attention to detail and accounting for additional sources of measurement uncertainty. The Pu-238 isotopic composition in New Brunswick Laboratory plutonium metal standard CRM 126-A was determined by thermal ionization mass spectrometry using combined Faraday cup and ion counting detection. A dynamic acquisition scheme was employed which provided for near real-time mass fractionation correction and ion counter/Faraday detector inter-calibration. Steps taken to minimize or eliminate isobaric U-238 interferences will be described, and an evaluation detailing contributions to the uncertainty, including SEM non-linearity, will be presented.

  9. Plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Miner, William N

    1964-01-01

    This pamphlet discusses plutonium from discovery to its production, separation, properties, fabrication, handling, and uses, including use as a reactor fuel and use in isotope power generators and neutron sources.

  10. Radiolysis of Salts and Long-Term Storage Issues for Both Pure and Impure PuO{sub 2} Materials in Plutonium Storage Containers

    Energy Technology Data Exchange (ETDEWEB)

    Lav Tandon

    2000-05-01

    The Material Identification and Surveillance (MIS) project sponsored a literature search on the effects of radiation on salts, with focus on alkali chlorides. The goal of the survey was to provide a basis for estimating the magnitude of {alpha} radiation effects on alkali chlorides that can accompany plutonium oxide (PuO{sub 2}) into storage. Chloride radiolysis can yield potentially corrosive gases in plutonium storage containers that can adversely affect long-term stability. This literature search was primarily done to provide a tutorial on this topic, especially for personnel with nonradiation chemistry backgrounds.

  11. Is Octavalent Pu(VIII) Possible? Mapping the Plutonium Oxyfluoride Series PuO(n)F(8-2n) (n = 0-4).

    Science.gov (United States)

    Huang, Wei; Pyykkö, Pekka; Li, Jun

    2015-09-01

    While the oxidation state Pu(VIII) is shown to be less stable than Pu(V) in the PuO4 molecule, it is not clear if the more electronegative fluorine can help to stabilize Pu(VIII). Our calculations on PuO(n)F(8-2n) (n = 0-4) molecules notably confirm that PuO2F4 has both (1)D(4h) and (5)C(2v) minima with the oxidation states Pu(VIII) and Pu(V), respectively, with the latter having lower energy. The hybrid-DFT, CCSD(T), and CASSCF methods all give the same result. The results conform to a superoxide ligand when n ≥ 2. PuF8 in a (1)O(h) state can decompose to PuF6 and F2, and PuOF6 in a (1)C(2v) state also can break down to PuF6 and 1/2 O2. The Pu(VIII) anion PuO2F5(-) does have a D(5h) minimum, which also lies above a (5)C(2v) Pu(V) peroxide structure. However, the energy differences between the different minima are not large, indicating that metastable species with oxidation states higher than Pu(V) cannot be completely excluded.

  12. Plutonium and the risk of cancer. A comparative analysis of Pu-body burdens due to releases from nuclear plants (Chelyabinsk-65, Gomel area) and global fallout.

    Science.gov (United States)

    Hohryakov, V F; Syslova, C G; Skryabin, A M

    1994-03-01

    Results of the analysis of dynamic body burdens of Pu in adult inhabitants of Chelyabinsk-65 (not occupationally exposed) and different areas of the Gomel region are presented for 1990-1991. The data are based on radiochemical analyses of Pu in human organs and tissues. Comparison with the published data on global Pu and our data for human autopsies (Ufa, Russia) revealed that estimates of Pubody burdens in Chelyabinsk-65 residents were up to 30 times higher than global levels and depended on the period of residence in town. The Pu body contents of Gomel citizens 4-5 years after the Chernobyl accident are on average 3-4 times higher than the global levels. Activity of Pu-238 in various organs constitutes 4.7-26.0% (on the average 13.5 +/- 5.0%) of the total alpha-activity of Pu-238 and Pu-239, 240. The expected number of cancers induced by incorporated plutonium is approximately the same for the two population groups despite their different sizes and does not differ from the global level by more than one order of magnitude.

  13. Plutonium

    Science.gov (United States)

    Clark, David L.; Hecker, Siegfried S.; Jarvinen, Gordon D.; Neu, Mary P.

    The element plutonium occupies a unique place in the history of chemistry, physics, technology, and international relations. After the initial discovery based on submicrogram amounts, it is now generated by transmutation of uranium in nuclear reactors on a large scale, and has been separated in ton quantities in large industrial facilities. The intense interest in plutonium resulted fromthe dual-use scenario of domestic power production and nuclear weapons - drawing energy from an atomic nucleus that can produce a factor of millions in energy output relative to chemical energy sources. Indeed, within 5 years of its original synthesis, the primary use of plutonium was for the release of nuclear energy in weapons of unprecedented power, and it seemed that the new element might lead the human race to the brink of self-annihilation. Instead, it has forced the human race to govern itself without resorting to nuclear war over the past 60 years. Plutonium evokes the entire gamut of human emotions, from good to evil, from hope to despair, from the salvation of humanity to its utter destruction. There is no other element in the periodic table that has had such a profound impact on the consciousness of mankind.

  14. {sup 239,} {sup 240,} {sup 241}Pu fingerprinting of plutonium in western US soils using ICPMS: solution and laser ablation measurements

    Energy Technology Data Exchange (ETDEWEB)

    Cizdziel, James V. [University of Nevada - Las Vegas, Harry Reid Center for Environmental Studies, Las Vegas, NV (United States); Ketterer, Michael E. [Northern Arizona University, Department of Chemistry and Biochemistry, Box 5698, Flagstaff, AZ (United States); Farmer, Dennis [University of Nevada - Las Vegas, Department of Health Physics, Las Vegas, NV (United States); Faller, Scott H. [US Environmental Protection Agency, Radiation and Indoor Environments National Laboratory, Box 98517, Las Vegas, NV (United States); Hodge, Vernon F. [University of Nevada - Las Vegas, Department of Chemistry, Las Vegas, NV (United States)

    2008-01-15

    Sector field inductively coupled plasma mass spectrometry (SF-ICPMS) has been used with analysis of solution samples and laser ablation (LA) of electrodeposited alpha sources to characterize plutonium activities and atom ratios prevalent in the western USA. A large set of surface soils and attic dusts were previously collected from many locations in the states of Nevada, Utah, Arizona, and Colorado; specific samples were analyzed herein to characterize the relative contributions of stratospheric fallout vs. Nevada Test Site (NTS) plutonium. This study illustrates two different ICPMS-based analytical strategies that are successful in fingerprinting Pu in environmental soils and dusts. Two specific datasets have been generated: (1) soils are leached with HNO{sub 3}-HCl, converted into electrodeposited alpha sources, counted by alpha spectrometry, then re-analyzed using laser ablation SF-ICPMS; (2) samples are completely dissolved by treatment with HNO{sub 3}-HF-H{sub 3}BO{sub 3}, Pu fractions are prepared by extraction chromatography, and analyzed by SF-ICPMS. Optimal laser ablation and ICPMS conditions were determined for the re-analysis of archived alpha spectrometry ''planchette'' sources. The best ablation results were obtained using a large spot size (200 {mu}m), a defocused beam, full repetition rate (20 Hz) and scan rate (200 {mu}m s{sup -1}); LA-ICPMS data were collected with a rapid electrostatic sector scanning experiment. Less than 10% of the electroplated surface area is consumed in the LA-ICPMS analysis, which would allow for multiple re-analyses. Excellent agreement was found between {sup 239+240}Pu activities determined by LA-ICPMS vs. activity results obtained by alpha spectrometry for the same samples ten years earlier. LA-ICPMS atom ratios for {sup 240}Pu/{sup 239}Pu and {sup 241}Pu/{sup 239}Pu range from 0.038-0.132 and 0.00034-0.00168, respectively, and plot along a two-component mixing line ({sup 241}Pu/{sup 239}Pu = 0

  15. 75 FR 41850 - Amended Notice of Intent to Modify the Scope of the Surplus Plutonium Disposition Supplemental...

    Science.gov (United States)

    2010-07-19

    ... fabrication into mixed uranium-plutonium oxide (MOX) reactor fuel in the Mixed Oxide Fuel Fabrication Facility... will analyze the potential environmental impacts of using MOX fuel in up to five reactors owned by the... processed into MOX fuel or to change the annual throughput, annual environmental impacts, or the types...

  16. Plutonium immobilization plant using ceramic in existing facilities at the Savannah River site

    Energy Technology Data Exchange (ETDEWEB)

    DiSabatino, A., LLNL

    1998-06-01

    The Plutonium Immobilization Plant (PIP) accepts plutonium (Pu) from pit conversion and from non-pit sources, and through a ceramic immobilization process converts the plutonium into an immobilized form that can be disposed of in a high level waste (HLW) repository. This immobilization process is shown conceptually in Figure 1-1. The objective is to make an immobilized form, suitable for geologic disposal, in which the plutonium is as inherently unattractive and inaccessible as the plutonium in spent fuel from commercial reactors. The ceramic immobilization alternative presented in this report consists of first converting the surplus material to an oxide, followed by incorporating the plutonium oxide into a titanate-based ceramic material that is placed in metal cans.

  17. Influence of the allotropic beta to alpha transformation and of oxygen on the distribution of plutonium in Zr-Pu and Ti-Pu dilute alloys

    CERN Document Server

    Languille, A; Remy, C

    1972-01-01

    Ti-Pu, Zr-Pu and Ti-U alloys, annealed above the transformation point, can show major segregation after cooling. The segregations increase with oxygen content. Annealing at high temperatures followed by severe quenching can cause them to disappear. (7 refs).

  18. The United States Plutonium Balance, 1944 - 2009

    Energy Technology Data Exchange (ETDEWEB)

    None

    2012-06-01

    This report updates the report -Plutonium: The first 50 years- which was released by the U.S.Department of Energy (DOE) in 1996. The topic of both reports is plutonium, sometimes referred to as Pu-239, which is capable of sustaining a nuclear chain reaction and is used in nuclear weapons and for nuclear power production. This report updates 1994 data through 2009. The four most significant changes since 1994 include: (a) the completion of cleanup activities at the Rocky Flats Plant in 2005; (b) material consolidation and disposition activities, especially shipments from Hanford to the Savannah River Site; (c) the 2007 declaration of an additional 9.0 MT of weapons grade plutonium to be surplus to defense needs in the coming decades; and (d) the opening of the Waste Isolation Pilot Plant (WIPP) near Carlsbad, New Mexico in 1999.

  19. Study of the effect of (U{sub 0.8}Pu{sub 0.2})O{sub 2} Uranium-Plutonium mixed fuel fission products on a living organism

    Energy Technology Data Exchange (ETDEWEB)

    Baimukhanova, Ayagoz; Kim, Dmitriy [Dept. of Radiation Protection, Institute of Nuclear Physics of the Ministry of Energy of the Republic of Kazakhstan, Almaty (Kazakhstan); Zhumagulova, Roza; Tazhigulova, Bibnur; Zharaspayeva, Gulzhanar; Azhiyeva, Galiya [Faculty of Engineering Technologies, Infrastructure and Management, International Educational Corporation, Almaty (Kazakhstan)

    2016-08-15

    The article describes the results of experiments conducted on pigs to determine the effect of plutonium, which is the most radiotoxic and highly active element in the range of mixed fuel (U{sub 0.8}Pu{sub 0.2})O{sub 2} fission products, on living organisms. The results will allow empirical prediction of the emergency plutonium radiation dose for various organs and tissues of humans in case of an accident in a reactor running on mixed fuel (U{sub 0.8}Pu{sub 0.2})O{sub 2}.

  20. Cost-benefit analysis of unfired PuO/sub 2/ pellets as an alternative plutonium shipping form

    Energy Technology Data Exchange (ETDEWEB)

    Mishima, J.; Brackenbush, L.W.; Libby, R.A.; Soldat, K.L.; White, G.D.

    1983-10-01

    A limited cost-benefit evaluation was performed concerning use of unfired plutonium dioxide pellets as a shipping form. Two specific processing operations are required for this use, one to form the pellet (pelletizing) and a second to reconstitute an acceptable powder upon receipt (reconstitution). The direct costs for the pelletizing operation are approximately $208,000 for equipment and its installation and $122 per kg of plutonium processed (based upon a 20-kg plutonium/day facility). The direct costs for reconstitution are approximately $90,000 for equipment and its installation and $81 per kg of plutonium processed. The indirect cost considered was personnel exposure from these operations. Whole body exposures ranged from 0.04 man-rem per 100 kg of low-exposure plutonium reconstituted to 0.9 man-rem per 100 kg of average-exposure plutonium pelletized. Hand exposures were much higher - 17 man-rem power 100 kg of low-exposure plutonium reconstituted to 67 man-rem per 100 kg of average plutonium pelletized. The principal benefit is a potential twentyfold reduction of airborne release in the event of an accident. An experimental plan is outlined to fill the data gaps uncovered during this study in the areas of pelletizing and reconstitution process parameters and pellet response behavior to accident-generated stresses. A study to enhance the containment potential of the inner packaging used during shipment is also outlined.

  1. EIS Data Call Report: Plutonium immobilization plant using ceramic in new facilities at the Savannah River Site

    Energy Technology Data Exchange (ETDEWEB)

    DiSabatino, A.

    1998-06-01

    The Plutonium Immobilization Plant (PIP) accepts plutonium (Pu) from pit conversion and from non-pit sources and, through a ceramic immobilization process, converts the plutonium into an immobilized form that can be disposed of in a high level waste (HLW) repository. This immobilization process is shown conceptually in Figure 1-1. The objective is to make an immobilized form, suitable for geologic disposal, in which the plutonium is as inherently unattractive and inaccessible as the plutonium in spent fuel from commercial reactors. The ceramic immobilization alternative presented in this report consists of first converting the surplus material to an oxide, followed by incorporating the plutonium oxide into a titanate-based ceramic material that is placed in metal cans.

  2. Aqueous Solution Chemistry of Plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Clark, David L. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2014-01-28

    Things I have learned working with plutonium: Chemistry of plutonium is complex; Redox equilibria make Pu solution chemistry particularly challenging in the absence of complexing ligands; Understanding this behavior is key to successful Pu chemistry experiments; There is no suitable chemical analog for plutonium.

  3. Potential of Vetiveria zizanoides L. Nash for phytoremediation of plutonium ((239)Pu): Chelate assisted uptake and translocation.

    Science.gov (United States)

    Singh, Shraddha; Fulzele, D P; Kaushik, C P

    2016-10-01

    Plants have demonstrated a great potential to remove toxic elements from soils and solutions and been successfully used for phytoremediation of important radionuclides. Uptake potential of vetiver plants (V. zizanoides) for the remediation of (239)Pu in hydroponic and soil conditions was studied in the present work. High efficiency of V. zizanoides for the removal of (239)Pu was recorded with 66.2% being removed from the hydroponic solution after 30 days. However, remediation of (239)Pu from soil was limited. Remediation of (239)Pu from soil was increased with the addition of chelating agents citric acid (CA) and diethylenetriaminepentaacetic acid (DTPA). Accumulation of (239)Pu was recorded higher in roots than shoots, however its translocation from roots to shoots increased in the presence of chelators in hydroponic as well as soil conditions. DTPA was found more effective than CA showing higher translocation index (TI). Increase in TI was observed 8 and 6 times in the solution and soil respectively when plants were exposed to (239)Pu-DTPA in comparison to only (239)Pu. The present study demonstrates that V. zizanoides plant is a potential plant for phytoremediation of (239)Pu. Copyright © 2016 Elsevier Inc. All rights reserved.

  4. Seaborg's Plutonium ?

    CERN Document Server

    Norman, Eric B; Telhami, Kristina E

    2014-01-01

    Passive x-ray and gamma-ray analysis was performed on UC Berkeley's EH&S Sample S338. The object was found to contain Pu-239 and no other radioactive isotopes. The mass of Pu-239 contained in this object was determined to be 2.0 +- 0.3 micrograms. These observations are consistent with the identification of this object being the 2.77-microgram plutonium oxide sample described by Glenn Seaborg and his collaborators as the first sample of Pu-239 that was large enough to be weighed.

  5. Evaluation of Self-absorption Effect of α-rays Emitted Spontaneously in Plutonium Oxide%PuO2颗粒对自发α射线的能量自吸收效应评估研究

    Institute of Scientific and Technical Information of China (English)

    罗文; 祝小惠; 宋英明; 朱志超

    2016-01-01

    A sphere geometry model for plutonium oxide-based alpha emitter was setup. The range of alpha particle in plutonium oxide pellet versus its energy and the spectral distribution of alpha particle emerging from the emitter surface were calculated using Monte Carlo method combined with the empirical formula of range. The internal radiation dose resulted by self-absorption effect ofα-rays emitted spontaneously in plutonium oxide was investigated accordingly. The result shows that the larger particle size the plutonium oxide-based alpha emitter has, the more obvious the self-absorption effect is and the better the correction effect of the intake absorbed dose that effects on human lung has. For plutonium oxide pellet with its particle size exceeding 2 µm, the correction quantity is expected to be larger than 5%. Our work is beneficial for a precise evaluation of internal radiation dose induced by inhaled radioactive material and microdosimetry study in radionuclide tumor therapy.%构建PuO2颗粒状α发射体的球体几何模型,采用蒙特卡罗和射程经验公式模拟计算α射线在PuO2颗粒中的射程能量关系式及α射线从PuO2颗粒表面出射的能谱分布,研究因PuO2颗粒对自发α射线的能量自吸收效应导致的对人体内照射剂量评估的影响。研究结果表明,PuO2粒径越大,其对自发α射线的能量自吸收效应越明显,内照射剂量的修正效果越好;当PuO2粒径在2µm以上时,内照射剂量的修正效果大于5%。本研究的结果对吸入放射性物质所致人体内照射剂量的准确估算有重要的参考价值,并可应用于放射性核素肿瘤治疗等领域的微剂量学研究。

  6. Accumulation of polonium 210Po, uranium (234U and 238U and plutonium (238Pu and 239+240Pu in tissues and organs of deer Carvidae from northern Poland

    Directory of Open Access Journals (Sweden)

    Strumińska-Parulska D. I.

    2013-04-01

    Full Text Available Livers, kidneys and muscles of large herbivorous animals: roe deer (Capreolus capreolus, red deer (Cervus elaphus and fallow deer (Dama dama, collected in northern Poland, were the subject of the investigation. Polonium, uranium and plutonium activities were measured using alpha spectrometry along with relevant radiochemical procedures. The average concentrations of 210Po ranged between 0.02±0.01 Bq kg−1 ww in muscles and 7.15±0.12 Bq kg−1 ww in kidneys. The concentration of 238U ranged widely between 2.49±0.18 and 69.37±5.45 mBq kg−1 ww. The average concentrations of 239+240Pu ranged between 0.18±0.04 mBq kg−1 ww in muscle and 2.77±0.60 mBq kg−1 ww in kidneys. Statistical analysis showed that the sampling location, sex, age and species did not influence on the radioisotope activities in the analyzed samples.

  7. Aerosol Physics Considerations for Using Cerium Oxide CeO2 as a Surrogate for Plutonium Oxide PuO2 in Airborne Release Fraction Measurements for Storage Container Investigations

    Energy Technology Data Exchange (ETDEWEB)

    Moore, Murray E. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Tao, Yong [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2017-02-16

    Cerium oxide (CeO2) dust is recommended as a surrogate for plutonium oxide (PuO2) in airborne release fraction experiments. The total range of applicable particle sizes for PuO2 extends from 0.0032 μm (the diameter of a single PuO2 molecule) to 10 μm (the defined upper boundary for respirable particles). For particulates with a physical particle diameter of 1.0 μm, the corresponding aerodynamic diameters for CeO2 and PuO2 are 2.7 μm and 3.4 μm, respectively. Cascade impactor air samplers are capable of measuring the size distributions of CeO2 or PuO2 particulates. In this document, the aerodynamic diameters for CeO2 and PuO2 were calculated for seven different physical diameters (0.0032, 0.02, 0.11, 0.27, 1.0, 3.2, and 10 μm). For cascade impactor measurements, CeO2 and PuO2 particulates with the same physical diameter would be collected onto the same or adjacent collection substrates. The difference between the aerodynamic diameter of CeO2 and PuO2 particles (that have the same physical diameter) is 39% of the resolution of a twelve-stage MSP Inc. 125 cascade impactor, and 34% for an eight-stage Andersen impactor. An approach is given to calculate the committed effective dose (CED) coefficient for PuO2 aerosol particles, compared to a corresponding aerodynamic diameter of CeO2 particles. With this approach, use of CeO2 as a surrogate for PuO2 material would follow a direct conversion based on a molar equivalent. In addition to the analytical information developed for this document, several US national labs have published articles about the use of CeO2 as a PuO2 surrogate. Different physical and chemical aspects were considered by these investigators, including thermal properties, ceramic formulations, cold pressing, sintering, molecular reactions, and mass loss in high temperature gas flows. All of those US national lab studies recommended the use of CeO2 as a surrogate material for PuO2.

  8. PLUTONIUM ELECTROREFINING CELLS

    Science.gov (United States)

    Mullins, L.J. Jr.; Leary, J.A.; Bjorklund, C.W.; Maraman, W.J.

    1963-07-16

    Electrorefining cells for obtaining 99.98% plutonium are described. The cells consist of an impure liquid plutonium anode, a molten PuCl/sub 3/-- alkali or alkaline earth metal chloanode, a molten PuCl/sub 3/-alkali or alkaline earth metal chloride electrolyte, and a nonreactive cathode, all being contained in nonreactive ceramic containers which separate anode from cathode by a short distance and define a gap for the collection of the purified liquid plutonium deposited on the cathode. Important features of these cells are the addition of stirrer blades on the anode lead and a large cathode surface to insure a low current density. (AEC)

  9. Detection of plutonium isotopes at lowest quantities using in-source resonance ionization mass spectrometry.

    Science.gov (United States)

    Raeder, S; Hakimi, A; Stöbener, N; Trautmann, N; Wendt, K

    2012-11-01

    The in-source resonance ionization mass spectrometry technique was applied for quantification of ultratrace amounts of plutonium isotopes as a proof of principle study. In addition to an overall detection limit of 10(4) to 10(5) atoms, this method enables the unambiguous identification and individual quantification of the plutonium isotopes (238)Pu and (241)Pu which are of relevance for dating of radiogenic samples. Due to the element-selective ionization process, these isotopes can be measured even under a high surplus of isobaric contaminations from (238)U or (241)Am, which considerably simplifies chemical preparation. The technique was developed, tested, and characterized on a variety of synthetic and calibration samples and is presently applied to analyze environmental samples.

  10. Plutonium bioaccumulation in seabirds.

    Science.gov (United States)

    Strumińska-Parulska, Dagmara I; Skwarzec, Bogdan; Fabisiak, Jacek

    2011-12-01

    The aim of the paper was plutonium (²³⁸Pu and ²³⁹⁺²⁴⁰Pu) determination in seabirds, permanently or temporarily living in northern Poland at the Baltic Sea coast. Together 11 marine birds species were examined: 3 species permanently residing in the southern Baltic, 4 species of wintering birds and 3 species of migrating birds. The obtained results indicated plutonium is non-uniformly distributed in organs and tissues of analyzed seabirds. The highest plutonium content was found in the digestion organs and feathers, the smallest in skin and muscles. The plutonium concentration was lower in analyzed species which feed on fish and much higher in herbivorous species. The main source of plutonium in analyzed marine birds was global atmospheric fallout.

  11. Actinide Oxidation State and O/M Ratio in Hypostoichiometric Uranium-Plutonium-Americium U0.750Pu0.246Am0.004O2-x Mixed Oxides.

    Science.gov (United States)

    Vauchy, Romain; Belin, Renaud C; Robisson, Anne-Charlotte; Lebreton, Florent; Aufore, Laurence; Scheinost, Andreas C; Martin, Philippe M

    2016-03-07

    Innovative americium-bearing uranium-plutonium mixed oxides U1-yPuyO2-x are envisioned as nuclear fuel for sodium-cooled fast neutron reactors (SFRs). The oxygen-to-metal (O/M) ratio, directly related to the oxidation state of cations, affects many of the fuel properties. Thus, a thorough knowledge of its variation with the sintering conditions is essential. The aim of this work is to follow the oxidation state of uranium, plutonium, and americium, and so the O/M ratio, in U0.750Pu0.246Am0.004O2-x samples sintered for 4 h at 2023 K in various Ar + 5% H2 + z vpm H2O (z = ∼ 15, ∼ 90, and ∼ 200) gas mixtures. The O/M ratios were determined by gravimetry, XAS, and XRD and evidenced a partial oxidation of the samples at room temperature. Finally, by comparing XANES and EXAFS results to that of a previous study, we demonstrate that the presence of uranium does not influence the interactions between americium and plutonium and that the differences in the O/M ratio between the investigated conditions is controlled by the reduction of plutonium. We also discuss the role of the homogeneity of cation distribution, as determined by EPMA, on the mechanisms involved in the reduction process.

  12. Pu and Am determination in the environment—method development

    Science.gov (United States)

    Afonin, M.; Simonoff, M.; Donard, O.; Michel, H.; Ardisson, G.

    2003-01-01

    A high resolution inductively coupled plasma mass spectrometric (HR-ICP-MS) method for the determination of plutonium isotopes, Am and the 240Pu/239Pu isotope ratio utilising modification of Pu-02-RC Plutonium in Soil Samples, Pu-03-RC Plutonium in Soil Residue—Total Dissolution Method, Pu-11-RC Plutonium Purification—Ion Exchange Technique, Pu-12-RC Plutonium and/or Americium in Soil or Sediments, HASL-300 was developed. Total plutonium concentrations (239+240Pu) measured in environmental samples by this HR-ICP-MS method were in good agreement with recommended data obtained from a-spectrometry. It was achieved the decreasing of the time to analyze the samples over than 33%.

  13. Isotopic composition and distribution of plutonium in northern South China Sea sediments revealed continuous release and transport of Pu from the Marshall Islands.

    Science.gov (United States)

    Wu, Junwen; Zheng, Jian; Dai, Minhan; Huh, Chih-An; Chen, Weifang; Tagami, Keiko; Uchida, Shigeo

    2014-03-18

    The (239+240)Pu activities and (240)Pu/(239)Pu atom ratios in sediments of the northern South China Sea and its adjacent Pearl River Estuary were determined to examine the spatial and temporal variations of Pu inputs. We clarified that Pu in the study area is sourced from a combination of global fallout and close-in fallout from the Pacific Proving Grounds in the Marshall Islands where above-ground nuclear weapons testing was carried out during the period of 1952-1958. The latter source dominated the Pu input in the 1950s, as evidenced by elevated (240)Pu/(239)Pu atom ratios (>0.30) in a dated sediment core. Even after the 1950s, the Pacific Proving Grounds was still a dominant Pu source due to continuous transport of remobilized Pu from the Marshall Islands, about 4500 km away, along the North Equatorial Current followed by the transport of the Kuroshio current and its extension into the South China Sea through the Luzon Strait. Using a simple two end-member mixing model, we have quantified the contributions of Pu from the Pacific Proving Grounds to the northern South China Sea shelf and the Pearl River Estuary are 68% ± 1% and 30% ± 5%, respectively. This study also confirmed that there were no clear signals of Pu from the Fukushima Daiichi Nuclear Power Plant accident impacting the South China Sea.

  14. Plutonium Story

    Science.gov (United States)

    Seaborg, G. T.

    1981-09-01

    The first nuclear synthesis and identification (i.e., the discovery) of the synthetic transuranium element plutonium (isotope /sup 238/Pu) and the demonstration of its fissionability with slow neutrons (isotope /sup 239/Pu) took place at the University of California, Berkeley, through the use of the 60-inch and 37-inch cyclotrons, in late 1940 and early 1941. This led to the development of industrial scale methods in secret work centered at the University of Chicago's Metallurgical Laboratory and the application of these methods to industrial scale production, at manufacturing plants in Tennessee and Washington, during the World War II years 1942 to 1945. The chemical properties of plutonium, needed to devise the procedures for its industrial scale production, were studied by tracer and ultramicrochemical methods during this period on an extraordinarily urgent basis. This work, and subsequent investigations on a worldwide basis, have made the properties of plutonium very well known. Its well studied electronic structure and chemical properties give it a very interesting position in the actinide series of inner transition elements.

  15. Plutonium immobilization in glass and ceramics

    Energy Technology Data Exchange (ETDEWEB)

    Knecht, D.A. [Lockheed Martin Idaho Technologies, Idaho Falls (United States); Murphy, W.M. [Southwest Research Institute, San Antonio, TX (United States)

    1996-05-01

    The Materials Research Society Nineteenth Annual Symposium on the Scientific Basis for Nuclear Waste Management was held in Boston on November 27 to December 1, 1995. Over 150 papers were presented at the Symposium dealing with all aspects of nuclear waste management and disposal. Fourteen oral sessions and on poster session included a Plenary session on surplus plutonium dispositioning and waste forms. The proceedings, to be published in April, 1996, will provide a highly respected, referred compilation of the state of scientific development in the field of nuclear waste management. This paper provides a brief overview of the selected Symposium papers that are applicable to plutonium immobilization and plutonium waste form performance. Waste forms that were described at the Symposium cover most of the candidate Pu immobilization options under consideration, including borosilicate glass with a melting temperature of 1150 {degrees}C, a higher temperature (1450 {degrees}C) lanthanide glass, single phase ceramics, multi-phase ceramics, and multi-phase crystal-glass composites (glass-ceramics or slags). These Symposium papers selected for this overview provide the current status of the technology in these areas and give references to the relevant literature.

  16. SURPLUS DILEMMA

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    On top of yuan revaluation and a huge trade surplus, the Chinese Government must also address ballooning forex reserves At the end of 2005, China's foreign exchange surplus totaled $818.87 billion, a leap of $208.9 billion over the previous year and an amount that is expected to have topped Japan's to become the world's largest.

  17. Anaerobic Biotransformation and Mobility of Pu and Pu-EDTA

    Energy Technology Data Exchange (ETDEWEB)

    Bolton, H., Jr.; Rai, D.; Xun, L.

    2005-04-18

    The complexation of radionuclides (e.g., plutonium (Pu) and {sup 60}Co) by codisposed ethylenediaminetetraacetate (EDTA) has enhanced their transport in sediments at DOE sites. Our previous NABIR research investigated the aerobic biodegradation and biogeochemistry of Pu(IV)-EDTA. Plutonium(IV) forms stable complexes with EDTA under aerobic conditions and an aerobic EDTA degrading bacterium can degrade EDTA in the presence of Pu and decrease Pu mobility. However, our recent studies indicate that while Pu(IV)-EDTA is stable in simple aqueous systems, it is not stable in the presence of relatively soluble Fe(III) compounds (i.e., Fe(OH){sub 3}(s)--2-line ferrihydrite). Since most DOE sites have Fe(III) containing sediments, Pu(IV) in likely not the mobile form of Pu-EDTA in groundwater. The only other Pu-EDTA complex stable in groundwater relevant to DOE sites would be Pu(III)-EDTA, which only forms under anaerobic conditions. Research is therefore needed in this brand new project to investigate the biotransformation of Pu and Pu-EDTA under anaerobic conditions. The biotransformation of Pu and Pu-EDTA under various anaerobic regimes is poorly understood including the reduction kinetics of Pu(IV) to Pu(III) from soluble (Pu(IV)-EDTA) and insoluble Pu(IV) as PuO2(am) by metal reducing bacteria, the redox conditions required for this reduction, the strength of the Pu(III)-EDTA complex, how the Pu(III)-EDTA complex competes with other dominant anoxic soluble metals (e.g., Fe(II)), and the oxidation kinetics of Pu(III)-EDTA. Finally, the formation of a stable soluble Pu(III)-EDTA complex under anaerobic conditions would require degradation of the EDTA complex to limit Pu(III) transport in geologic environments. Anaerobic EDTA degrading microorganisms have not been isolated. These knowledge gaps preclude the development of a mechanistic understanding of how anaerobic conditions will influence Pu and Pu-EDTA fate and transport to assess, model, and design approaches to stop

  18. Simultaneous determination of radiocesium ((135)Cs, (137)Cs) and plutonium ((239)Pu, (240)Pu) isotopes in river suspended particles by ICP-MS/MS and SF-ICP-MS.

    Science.gov (United States)

    Cao, Liguo; Zheng, Jian; Tsukada, Hirofumi; Pan, Shaoming; Wang, Zhongtang; Tagami, Keiko; Uchida, Shigeo

    2016-10-01

    Due to radioisotope releases in the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, long-term monitoring of radiocesium ((135)Cs and (137)Cs) and Pu isotopes ((239)Pu and (240)Pu) in river suspended particles is necessary to study the transport and fate of these long-lived radioisotopes in the land-ocean system. However, it is expensive and technically difficult to collect samples of suspended particles from river and ocean. Thus, simultaneous determination of multi-radionuclides remains as a challenging topic. In this study, for the first time, we report an analytical method for simultaneous determination of radiocesium and Pu isotopes in suspended particles with small sample size (1-2g). Radiocesium and Pu were sequentially pre-concentrated using ammonium molybdophosphate and ferric hydroxide co-precipitation, respectively. After the two-stage ion-exchange chromatography separation from the matrix elements, radiocesium and Pu isotopes were finally determined by ICP-MS/MS and SF-ICP-MS, respectively. The interfering elements of U ((238)U(1)H(+) and (238)U(2)H(+) for (239)Pu and (240)Pu, respectively) and Ba ((135)Ba(+) and (137)Ba(+) for (135)Cs and (137)Cs, respectively) were sufficiently removed with the decontamination factors of 1-8×10(6) and 1×10(4), respectively, with the developed method. Soil reference materials were utilized for method validation, and the obtained (135)Cs/(137)Cs and (240)Pu/(239)Pu atom ratios, and (239+240)Pu activities showed a good agreement with the certified/information values. In addition, the developed method was applied to analyze radiocesium and Pu in the suspended particles of land water samples collected from Fukushima Prefecture after the FDNPP accident. The (135)Cs/(137)Cs atom ratios (0.329-0.391) and (137)Cs activities (23.4-152Bq/g) suggested radiocesium contamination of the suspended particles mainly originated from the accident-released radioactive contaminates, while similar Pu contamination of suspended

  19. Real-time monitoring of plutonium content in uranium-plutonium alloys

    Science.gov (United States)

    Li, Shelly Xiaowei; Westphal, Brian Robert; Herrmann, Steven Douglas

    2015-09-01

    A method and device for the real-time, in-situ monitoring of Plutonium content in U--Pu Alloys comprising providing a crucible. The crucible has an interior non-reactive to a metallic U--Pu alloy within said interior of said crucible. The U--Pu alloy comprises metallic uranium and plutonium. The U--Pu alloy is heated to a liquid in an inert or reducing atmosphere. The heated U--Pu alloy is then cooled to a solid in an inert or reducing atmosphere. As the U--Pu alloy is cooled, the temperature of the U--Pu alloy is monitored. A solidification temperature signature is determined from the monitored temperature of the U--Pu alloy during the step of cooling. The amount of Uranium and the amount of Plutonium in the U--Pu alloy is then determined from the determined solidification temperature signature.

  20. SRS vitrification studies in support of the U.S. program for disposition of excess plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Wicks, G.G.; McKibben, J.M.; Plodinec, M.J.; Ramsey, W.G.

    1995-09-01

    Many thousands of nuclear weapons are being retired in the U.S. and Russian as a result of nuclear disarmament activities. These efforts are expected to produce a surplus of about 50 MT of weapons grade plutonium (Pu) in each country. In addition to this inventory, the U.S. Department of Energy (DOE) has more than 20 MT of Pu scrap, residue, etc., and Russian is also believed to have at least as much of this type of material. The entire surplus Pu inventories in the U.S. and Russian present a clear and immediate danger to national and international security. It is important that a solution be found to secure and manage this material effectively and that such an effort be implemented as quickly as possible. One option under consideration is vitrification of Pu into a safe, durable, accountable and proliferation-resistant form. As a result of decades to experience within the DOE community involving vitrification of a variety of hazardous and radioactive wastes, this existing technology can now be expanded to include mobilization of large amounts of Pu. This technology can then be implemented rapidly using the many existing resources currently available. An overall strategy to vitrify many different types of Pu will be already developed throughout the waste management community can be used in a staged Pu vitrification effort. This approach uses the flexible vitrification technology already available and can even be made portable so that it may be brought to the source and ultimately, used to produce a consistent and common borosilicate glass composition for the vitrified Pu. The final composition of this product can be made similar to nationally and internationally accepted HLW glasses.

  1. Density of Plutonium Turnings Generated from Machining Activities

    Energy Technology Data Exchange (ETDEWEB)

    Gonzales, John Robert [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Vigil, Duane M. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Jachimowski, Thomas A. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Archuleta, Alonso [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Arellano, Gerald Joseph [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Melton, Vince Lee [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2016-10-20

    The purpose of this project was to determine the density of plutonium (Pu) turnings generated from the range of machining activities, using both surrogate material and machined Pu turnings. Verify that 500 grams (g) of plutonium will fit in a one quart container using a surrogate equivalent volume and that 100 grams of Pu will fit in a one quart Savy container.

  2. Plutonium Oxide Process Capability Work Plan

    Energy Technology Data Exchange (ETDEWEB)

    Meier, David E. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Tingey, Joel M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2014-02-28

    Pacific Northwest National Laboratory (PNNL) has been tasked to develop a Pilot-scale Plutonium-oxide Processing Unit (P3U) providing a flexible capability to produce 200g (Pu basis) samples of plutonium oxide using different chemical processes for use in identifying and validating nuclear forensics signatures associated with plutonium production. Materials produced can also be used as exercise and reference materials.

  3. Analysis Method of 241Pu Radioactivity by Isotope Dilution-Extraction Liquid Scintillation Spectrometer

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    <正>241Pu is the only pure β emitter with the maximum energy of 20.81 keV in plutonium isotopes of 238Pu, 239Pu, 240Pu and 242Pu, in which 241Pu is mostly specific radioactivity because its half-life is 14.29 a.

  4. Influence of humic acid on plutonium sorption to gibbsite. Determination of Pu-humic acid complexation constants and ternary sorption studies

    Energy Technology Data Exchange (ETDEWEB)

    Zimmerman, Trevor; Powell, Brian A. [Clemson Univ., Anderson, SC (United States). Environmental Engineering and Earth Sciences; Zavarin, Mavrik [Lawrence Livermore National Laboratory, Livermore, CA (United States). Glenn T. Seaborg Institute

    2014-10-01

    In this work stability constants describing Pu(IV), Th(IV), and Np(V) binding to Leonardite humic acid (HA) were determined using a discrete pK{sub a} model. A hybrid ultra-filtration/equilibrium dialysis, ligand exchange technique was used to generate the partitioning data. Ethylenediaminetetraacetic acid (EDTA) was used as a reference ligand to allow the aqueous chemistry of the Pu(IV)-HA system to be examined over a range of pH values, while minimizing the possibility of precipitation of Pu(IV). The conditional stability constant for Pu(IV) complexation with HA determined as part of this work is logβ{sub 112} = 6.76 ± 0.14 based on the equation: Pu{sup 4+} + HL3 + 2H{sub 2}O <-> Pu(OH){sub 2}L3{sup +} + 3H{sup +} where HA is represented by HL3 (a binding site on the HA with a pK{sub a} value of 7). This value is three orders of magnitude higher than the Th(IV)-HA constant and between six and eight orders of magnitude higher than the Np(V)-HA complex. The magnitude of the stability constants and the general trend of increasing complexation strength with increasing pH is consistent with previous observations. The Pu(IV)-HA stability constants were used to model sorption of Pu(IV) to gibbsite in the presence of HA. Assuming only aqueous Pu-HA complexes and AlOH-Pu surface complexes, the model was unable to predict the observed data which exhibited greater sorption at pH 4 relative to pH 6; a phenomenon which does not occur in the absence of HA. Therefore, this study demonstrates that ternary Pu-HA-gibbsite complexes may form under low pH conditions and exhibit greater sorption than that observed in the absence of HA. Although the presence of HA may increase the solubility/aqueous concentrations of Pu in the absence of a solid phase, formation of ternary complexes may indeed retard the subsurface migration of Pu. The corollary to this finding is that increased mobility may occur if the ternary surface complex forms on a mobile colloid rather than part of the

  5. Analysis of {sup 236}U and plutonium isotopes, {sup 239,240}Pu, on the 1 MV AMS system at the Centro Nacional de Aceleradores, as a potential tool in oceanography

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, Elena; López-Lora, Mercedes [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Villa, María [Departamento de Física Aplicada II, Universidad de Sevilla, Av. Reina Mercedes 4A, 41012 Seville (Spain); Servicio de Radioisótopos, Centro de Investigación, Tecnología e Innovación, Universidad de Sevilla, Av. Reina Mercedes 4B, 41012 Seville (Spain); Casacuberta, Núria [Laboratory of Ion Beam Physics, ETH Zürich, Otto-Stern-Weg 5, CH-8093 Zürich (Switzerland); López-Gutiérrez, José María [Centro Nacional de Aceleradores (Universidad de Sevilla, Consejo Superior de Investigaciones Científicas, Junta de Andalucía), Thomas Alva Edison 7, 41092 Seville (Spain); Departamento de Física Aplicada I, Escuela Universitaria Politécnica, Universidad de Sevilla, Virgen de África 7, 41011 Seville (Spain); Pham, Mai Khanh [IAEA-Environment Laboratories, Monte Carlo 98000 (Monaco)

    2015-10-15

    The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for {sup 236}U and {sup 239,240}Pu measurements has been extensively investigated. A very promising {sup 236}U/{sup 238}U abundance sensitivity of about 3 × 10{sup −11} has been recently achieved, and background figures for {sup 239}Pu of about 10{sup 6} atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of {sup 236}U and {sup 239}Pu and its further application in environmental studies. First {sup 236}U results obtained on our AMS system for marine samples (sediments and water) are presented here. Results of two new IAEA reference materials (IAEA-410 and IAEA-412, marine sediments from Pacific Ocean) are reported. The obtained {sup 236}U/{sup 239}Pu atom ratios, of 0.12 and 0.022, respectively, show a dependency with the contamination source (i.e. local fallout from the US tests performed at the Bikini Atoll and general fallout). The results obtained for a third IAEA reference material (IAEA-381, seawater from the Irish Sea), are also presented. In the following, the uranium and plutonium isotopic compositions obtained on a set of 5 intercomparison seawater samples from the Arctic Ocean provided by the ETH Zürich are discussed. By comparing them with the obtained results on the 600 kV AMS facility Tandy at the ETH Zürich, we demonstrate the solidity of the CNA technique for {sup 236}U/{sup 238}U determinations at, at least, 7 × 10{sup −10} level. Finally, these results are discussed in their environmental context.

  6. Plutonium isotope ratio variations in North America

    Energy Technology Data Exchange (ETDEWEB)

    Steiner, Robert E [Los Alamos National Laboratory; La Mont, Stephen P [Los Alamos National Laboratory; Eisele, William F [Los Alamos National Laboratory; Fresquez, Philip R [Los Alamos National Laboratory; Mc Naughton, Michael [Los Alamos National Laboratory; Whicker, Jeffrey J [Los Alamos National Laboratory

    2010-12-14

    Historically, approximately 12,000 TBq of plutonium was distributed throughout the global biosphere by thermo nuclear weapons testing. The resultant global plutonium fallout is a complex mixture whose {sup 240}Pu/{sup 239}Pu atom ratio is a function of the design and yield of the devices tested. The average {sup 240}Pu/{sup 239}Pu atom ratio in global fallout is 0.176 + 014. However, the {sup 240}Pu/{sup 239}Pu atom ratio at any location may differ significantly from 0.176. Plutonium has also been released by discharges and accidents associated with the commercial and weapons related nuclear industries. At many locations contributions from this plutonium significantly alters the {sup 240}Pu/{sup 239}Pu atom ratios from those observed in global fallout. We have measured the {sup 240}Pu/{sup 239}Pu atom ratios in environmental samples collected from many locations in North America. This presentation will summarize the analytical results from these measurements. Special emphasis will be placed on interpretation of the significance of the {sup 240}Pu/{sup 239}Pu atom ratios measured in environmental samples collected in the Arctic and in the western portions of the United States.

  7. Electrochemically Modulated Separation for Plutonium Safeguards

    Energy Technology Data Exchange (ETDEWEB)

    Pratt, Sandra H.; Breshears, Andrew T.; Arrigo, Leah M.; Schwantes, Jon M.; Duckworth, Douglas C.

    2013-12-31

    Accurate and timely analysis of plutonium in spent nuclear fuel is critical in nuclear safeguards for detection of both protracted and rapid plutonium diversions. Gamma spectroscopy is a viable method for accurate and timely measurements of plutonium provided that the plutonium is well separated from the interfering fission and activation products present in spent nuclear fuel. Electrochemically modulated separation (EMS) is a method that has been used successfully to isolate picogram amounts of Pu from nitric acid matrices. With EMS, Pu adsorption may be turned "on" and "off" depending on the applied voltage, allowing for collection and stripping of Pu without the addition of chemical reagents. In this work, we have scaled up the EMS process to isolate microgram quantities of Pu from matrices encountered in spent nuclear fuel during reprocessing. Several challenges have been addressed including surface area limitations, radiolysis effects, electrochemical cell performance stability, and chemical interferences. After these challenges were resolved, 6 µg Pu was deposited in the electrochemical cell with approximately an 800-fold reduction of fission and activation product levels from a spent nuclear fuel sample. Modeling showed that these levels of Pu collection and interference reduction may not be sufficient for Pu detection by gamma spectroscopy. The main remaining challenges are to achieve a more complete Pu isolation and to deposit larger quantities of Pu for successful gamma analysis of Pu. If gamma analyses of Pu are successful, EMS will allow for accurate and timely on-site analysis for enhanced Pu safeguards.

  8. Stop plutonium; Stop plutonium

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2003-02-01

    This press document aims to inform the public on the hazards bound to the plutonium exploitation in France and especially the plutonium transport. The first part is a technical presentation of the plutonium and the MOX (Mixed Oxide Fuel). The second part presents the installation of the plutonium industry in France. The third part is devoted to the plutonium convoys safety. The highlight is done on the problem of the leak of ''secret'' of such transports. (A.L.B.)

  9. Ultra-Small Plutonium Oxide Nanocrystals: An Innovative Material in Plutonium Science

    OpenAIRE

    HUDRY DAMIEN; Griveau, Jean-Christophe; Apostolidis, Christos; WALTER OLAF; Janssen, Arne; Manara, Dario; Colineau, Eric; VITOVA T.; Wang, Di; KUEBEL Christian; MEYER D.j.m.

    2013-01-01

    Apart from its sensitive technological importance, plutonium (Pu) is also one of the most intriguing elements because of its non-conventional physical properties and fascinating chemistry. Those fundamental aspects are particularly interesting when dealing with the challenging study of plutonium-based nanomaterials. Here we show that ultra-small (3.2  0.9 nm) and highly crystalline plutonium oxide (PuO2) nanocrystals (NCs) can be synthesized by the thermal decomposition of plutonyl nitrate (...

  10. The solubility of hydrogen and deuterium in alloyed, unalloyed and impure plutonium metal

    Energy Technology Data Exchange (ETDEWEB)

    Richmond, Scott [Los Alamos National Laboratory; Bridgewater, Jon S [Los Alamos National Laboratory; Ward, John W [Los Alamos National Laboratory; Allen, Thomas A [Los Alamos National Laboratory

    2009-01-01

    Pressure-Composition-Temperature (PCT) data are presented for the plutonium-hydrogen (Pu-H) and plutonium-deuterium (Pu-D) systems in the solubility region up to terminal solubility (precipitation of PuH{sub 2}). The heats of solution for PuH{sub s} and PuD{sub s} are determined from PCT data in the ranges 350-625 C for gallium alloyed Pu and 400-575 C for unalloyed Pu. The solubility of high purity plutonium alloyed with 2 at.% gallium is compared to high purity unalloyed plutonium. Significant differences are found in hydrogen solubility for unalloyed Pu versus gallium alloyed Pu. Differences in hydrogen solubility due to an apparent phase change are observable in the alloyed and unalloyed solubilities. The effect of iron impurities on Pu-Ga alloyed Pu is shown via hydrogen solubility data as preventing complete homogenization.

  11. Report of an investigation into deterioration of the Plutonium Fuel Form Fabrication Facility (PuFF) at the DOE Savannah River Site

    Energy Technology Data Exchange (ETDEWEB)

    1991-10-01

    This investigations of the Savannah River Site's Plutonium Fuel Form fabrication facility located in Building 235-F was initiated in April 1991. The purpose of the investigation was to determine whether, as has been alleged, operation of the facility's argon inert gas system was terminated with the knowledge that continued inoperability of the argon system would cause accelerated corrosion damage to the equipment in the plutonium 238 processing cells. The investigation quickly established that the decision to discontinue operation of the argon system, by not repairing it, was merely one of the measures, and not the most important one, which led to the current deteriorated state of the facility. As a result, the scope of the investigation was broadened to more identify and assess those factors which contributed to the facility's current condition. This document discusses the backgrounds, results, and recommendations of this investigation.

  12. A mechanism for plutonium pyrophoricity

    Science.gov (United States)

    Martz, Joseph C.; Haschke, John M.; Stakebake, Jerry L.

    1994-06-01

    A proposed mechanism for plutonium pyrophoricity quantitatively predicts the ignition temperature of plutonium as a function of surface : mass ratio and particle size. Plutonium must exceed 475°C before self-ignition occurs. External heating of massive samples is necessary to achieve this condition, while finely divided materials can reach the ignition point by an alternative, two-step mechanism. First, the thin layer of surface PuO 2 on the metal undergoes kinetically controlled reduction to Pu 2O 3 near 150°C. Second, the trivalent Pu 2O 3 reacts with gas-phase oxygen to reform PuO 2. Heat generated from the second reaction is sufficient to raise the temperature of small particles or thin foils above the 475°C ignition point. Details of this mechanism are given, including a discussion of plutonium oxidation and a calculation of adiabatic temperature increase due to oxidation of the Pu 2O 3 surface layer. Plutonium pyrophoricity data are summarized and compared to model results.

  13. Surprising coordination for plutonium in the first plutonium(III) borate.

    Science.gov (United States)

    Wang, Shuao; Alekseev, Evgeny V; Depmeier, Wulf; Albrecht-Schmitt, Thomas E

    2011-03-21

    The first plutonium(III) borate, Pu(2)[B(12)O(18)(OH)(4)Br(2)(H(2)O)(3)]·0.5H(2)O, has been prepared by reacting plutonium(III) with molten boric acid under strictly anaerobic conditions. This compound contains a three-dimensional polyborate network with triangular holes that house the plutonium(III) sites. The plutonium sites in this compound are 9- and 10-coordinate and display atypical geometries.

  14. Accelerator mass spectrometry (AMS) in plutonium analysis.

    Science.gov (United States)

    Strumińska-Parulska, Dagmara I

    The paper summarizes the results of the (240)Pu/(239)Pu atomic ratio studies in atmospheric fallout samples collected in 1986 over Gdynia (Poland) as well as three Baltic fish species collected in 1997 using the accelerator mass spectrometry. A new generation of AMS has been developed during last years and this method is an efficient and good technique to measure long-lived radioisotopes in the environment and provides the most accurate determination of the atomic ratios between (240)Pu and (239)Pu. The nuclide compositions of plutonium in filter samples correspond to their means of production. AMS measurements of atmospheric fallout collected in April showed sufficient increase of the (240)Pu/(239)Pu atomic ratio from 0.28 from March to 0.47. Also such high increase of (240)Pu/(239)Pu atomic ratio, close to reactor core (240)Pu/(239)Pu atomic ratio, was observed in September and equaled 0.47.

  15. Determination by gamma-ray spectrometry of the plutonium and americium content of the Pu/Am separation scraps. Application to molten salts; Determination par spectrometrie gamma de la teneur en plutonium et en americium de produits issus de separation Pu/Am. Application aux bains de sels

    Energy Technology Data Exchange (ETDEWEB)

    Godot, A. [CEA Valduc, Dept. de Traitement des Materiaux Nucleaires, 21 - Is-sur-Tille (France); Perot, B. [CEA Cadarache, Dept. de Technologie Nucleaire, Service de Modelisation des Transferts et Mesures Nucleaires, 13 - Saint-Paul-lez-Durance (France)

    2005-07-01

    Within the framework of plutonium recycling operations in CEA Valduc (France), americium is extracted from molten plutonium metal into a molten salt during an electrolysis process. The scraps (spent salt, cathode, and crucible) contain extracted americium and a part of plutonium. Nuclear material management requires a very accurate determination of the plutonium content. Gamma-ray spectroscopy is performed on Molten Salt Extraction (MSE) scraps located inside the glove box, in order to assess the plutonium and americium contents. The measurement accuracy is influenced by the device geometry, nuclear instrumentation, screens located between the sample and the detector, counting statistics and matrix attenuation, self-absorption within the spent salt being very important. The purpose of this study is to validate the 'infinite energy extrapolation' method employed to correct for self-attenuation, and to detect any potential bias. We present a numerical study performed with the MCNP computer code to identify the most influential parameters and some suggestions to improve the measurement accuracy. A final uncertainty of approximately 40% is achieved on the plutonium mass. (authors)

  16. Plutonium in the marine environment at Thule, NW-Greenland after a nuclear weapons accident

    DEFF Research Database (Denmark)

    Dahlgaard, H.; Eriksson, M.; Ilus, E.

    2001-01-01

    than in sediments. Some biota groups show a somewhat higher uptake of americium than of plutonium. Sediment samples with weapons plutonium from the accident show a significant variation in Pu-240/Pu-239 atom ratios in the range 0.027-0.057. This supports the hypothesis that the Thule plutonium...

  17. 10 CFR 71.23 - General license: Plutonium-beryllium special form material.

    Science.gov (United States)

    2010-01-01

    ... 10 Energy 2 2010-01-01 2010-01-01 false General license: Plutonium-beryllium special form material... RADIOACTIVE MATERIAL General Licenses § 71.23 General license: Plutonium-beryllium special form material. (a... form of plutonium-beryllium (Pu-Be) special form sealed sources, or to deliver Pu-Be sealed sources...

  18. Alternating layers of plutonium and lead or indium as surrogate for plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Rudin, Sven P, E-mail: srudin@lanl.gov [Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)

    2010-03-15

    Elemental plutonium (Pu) assumes more crystal structures than other elements, plausibly due to bonding f electrons becoming non-bonding. Complex geometries hamper understanding of the transition in Pu, but calculations predict this transition in a system with simpler geometry: alternating layers either of plutonium and lead or of plutonium and indium. Here the transition occurs via a pairing-up of atoms within Pu layers. Calculations stepping through this pairing-up reveal valuable details of the transition, for example that the transition from bonding to non-bonding proceeds smoothly.

  19. Alternating layers of plutonium and lead or indium as surrogate for plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Rudin, Sven Peter [Los Alamos National Laboratory

    2009-01-01

    Elemental plutonium (Pu) assumes more crystal structures than other elements, plausibly due to bonding f electrons becoming non-bonding. Complex geometries hamper understanding of the transition in Pu, but calculations predict this transition in a system with simpler geometry: alternating layers either of plutonium and lead or of plutonium and indium. Here the transition occurs via a pairing-up of atoms within Pu layers. Calculations stepping through this pairing-up reveal valuable details of the transition, for example that the transition from bonding to non-bonding proceeds smoothly.

  20. Plutonium uptake by the green alga Scenedesmus obliquus (Turp) Kutz, as a function of isotope and oxidation state

    Energy Technology Data Exchange (ETDEWEB)

    Tkacik, M.F.

    1977-01-01

    This study was designed to determine the effect of plutonium chemical valence state on the availability of small concentrations of /sup 238/Pu and /sup 239/Pu to algae. The uptake experiments involved the green alga Scenedesmus obliquus, grown in batch cultures. Plutonium concentrations accumulated by this alga were linearly related to plutonium concentrations. There was no significant difference (rho = 0.05) in algal plutonium accumulations, on a mass basis, of either /sup 238/Pu or /sup 239/Pu in either Pu/sup +4/ or Pu/sup +6/ oxidation state at the concentrations studied.

  1. Plutonium, (137)Cs and uranium isotopes in Mongolian surface soils.

    Science.gov (United States)

    Hirose, K; Kikawada, Y; Igarashi, Y; Fujiwara, H; Jugder, D; Matsumoto, Y; Oi, T; Nomura, M

    2017-01-01

    Plutonium ((238)Pu and (239,240)Pu), (137)Cs and plutonium activity ratios ((238)Pu/(239,240)Pu) as did uranium isotope ratio ((235)U/(238)U) were measured in surface soil samples collected in southeast Mongolia. The (239,240)Pu and (137)Cs concentrations in Mongolian surface soils (surface soils (0.013-0.06) coincided with that of global fallout. The (235)U/(238)U atom ratios in the surface soil show the natural one. There was a good correlation between the (239,240)Pu and (137)Cs concentrations in the surface soils. We introduce the migration depth to have better understanding of migration behaviors of anthropogenic radionuclides in surface soil. We found a difference of the migration behavior between (239,240)Pu and (137)Cs from (137)Cs/(239,240)Pu - (137)Cs plots for the Mongolian and Tsukuba surface soils; plutonium in surface soil is migrated easier than (137)Cs.

  2. Adjustment of a direct method for the determination of man body burden in Pu-239 on by X-ray detection of U-235; Mise au point d'une methode directe de determination de la charge corporelle en plutonium 239 chez l'homme par detection X de l'uranium 235

    Energy Technology Data Exchange (ETDEWEB)

    Boulay, P. [Commissariat a l' Energie Atomique, Bruyeres-le-Chatel (France). Centre d' Etudes

    1968-04-01

    The use of Pu-239 on a larger scale sets a problem about the contamination measurement by aerosol at lung level. A method of direct measurement of Pu-239 lung burden is possible, thanks to the use of a large area window proportional counter. A counter of such pattern, has been especially carried out for this purpose. The adjustment of the apparatus allows an adequate sensibility to detect a contamination at the maximum permissible body burden level. Besides, a method for individual 'internal calibration', with a plutonium mock: the protactinium-233, is reported. (author) [French] L'utilisation a une echelle de plus en plus large du plutonium-239 pose un probleme de la mesure de la contamination par aerosol au niveau du poumon. Une methode de mesure directe de la charge pulmonaire en plutonium-239 est possible grace a l'utilisation d'un compteur proportionnel a fenetre de grande surface. Un compteur de ce type a specialement ete realise dans ce but. La mise au point de l'appareillage permet une sensibilite suffisante pour deceler une contamination au niveau de la Q.M.A (quantite maximale admissible). D'autre part, une methode 'd'etalonnage interne' de l'individu a l'aide d'un simulateur de plutonium, le protactinium-233, est decrite. (auteur)

  3. Elastic properties of Pu metal and Pu-Ga alloys

    Energy Technology Data Exchange (ETDEWEB)

    Soderlind, P; Landa, A; Klepeis, J E; Suzuki, Y; Migliori, A

    2010-01-05

    We present elastic properties, theoretical and experimental, of Pu metal and Pu-Ga ({delta}) alloys together with ab initio equilibrium equation-of-state for these systems. For the theoretical treatment we employ density-functional theory in conjunction with spin-orbit coupling and orbital polarization for the metal and coherent-potential approximation for the alloys. Pu and Pu-Ga alloys are also investigated experimentally using resonant ultrasound spectroscopy. We show that orbital correlations become more important proceeding from {alpha} {yields} {beta} {yields} {gamma} plutonium, thus suggesting increasing f-electron correlation (localization). For the {delta}-Pu-Ga alloys we find a softening with larger Ga content, i.e., atomic volume, bulk modulus, and elastic constants, suggest a weakened chemical bonding with addition of Ga. Our measurements confirm qualitatively the theory but uncertainties remain when comparing the model with experiments.

  4. Elastic properties of Pu metal and Pu-Ga alloys

    Science.gov (United States)

    Söderlind, Per; Landa, Alex; Klepeis, J. E.; Suzuki, Y.; Migliori, A.

    2010-06-01

    We present elastic properties, theoretical and experimental, of Pu metal and Pu-Ga (δ) alloys together with ab initio equilibrium equation of state for these systems. For the theoretical treatment we employ density-functional theory in conjunction with spin-orbit coupling and orbital polarization for the metal and coherent-potential approximation for the alloys. Pu and Pu-Ga alloys are also investigated experimentally using resonant ultrasound spectroscopy. We show that orbital correlations become more important proceeding from α→β→γ plutonium, thus suggesting increasing f -electron correlation and a corresponding softening of the elastic moduli. For the δ-Pu-Ga alloys we find a softening with larger Ga content, i.e., atomic volume, bulk modulus, and elastic constants imply a weakened chemical bonding with addition of Ga. Our measurements confirm qualitatively the theory but uncertainties remain when comparing the model with experiments.

  5. Plutonium speciation affected by environmental bacteria

    Energy Technology Data Exchange (ETDEWEB)

    Neu, M.P.; Icopini, G.A.; Boukhalfa, H. [Chemistry Div., C-SIC, Los Alamos National Lab., Los Alamos, NM (United States)

    2005-07-01

    Plutonium has no known biological utility, yet it has the potential to interact with bacterial cellular and extracellular structures that contain metal-binding groups, to interfere with the uptake and utilization of essential elements, and to alter cell metabolism. These interactions can transform plutonium from its most common forms, solid, mineral-adsorbed, or colloidal Pu(IV), to a variety of biogeochemical species that have much different physico-chemical properties. Organic acids that are extruded products of cell metabolism can solubilize plutonium and then enhance its environmental mobility, or in some cases facilitate plutonium transfer into cells. Phosphate- and carboxylate-rich polymers associated with cell walls can bind plutonium to form mobile biocolloids or Pu-laden biofilm/mineral solids. Bacterial membranes, proteins or redox agents can produce strongly reducing electrochemical zones and generate molecular Pu(III/IV) species or oxide particles. Alternatively, they can oxidize plutonium to form soluble Pu(V) or Pu(VI) complexes. This paper reviews research on plutonium-bacteria interactions and closely related studies on the biotransformation of uranium and other metals. (orig.)

  6. Aqueous Chloride Operations Overview: Plutonium and Americium Purification/Recovery

    Energy Technology Data Exchange (ETDEWEB)

    Kimball, David Bryan [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Skidmore, Bradley Evan [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2016-06-22

    Acqueous Chloride mission is to recover plutonium and americium from pyrochemical residues (undesirable form for utilization and storage) and generate plutonium oxide and americium oxide. Plutonium oxide is recycled into Pu metal production flowsheet. It is suitable for storage. Americium oxide is a valuable product, sold through the DOE-OS isotope sales program.

  7. Historical changes in 239Pu and 240Pu sources in sedimentary records in the East China Sea: Implications for provenance and transportation

    DEFF Research Database (Denmark)

    Wang, Jinlong; Baskaran, Mark; Hou, Xiaolin

    2017-01-01

    Concentrations and isotopic compositions of plutonium (Pu) are widely used for its source identification and to determine transport processes of Pu-associated particulate matter and water. We investigated the concentrations of 239Pu and 240Pu and their ratios in a number of sediment samples from...

  8. PU-ICE Summary Information.

    Energy Technology Data Exchange (ETDEWEB)

    Moore, Michael [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2017-05-01

    The Generator Knowledge Report for the Plutonium Isentropic Compression Experiment Containment Systems (GK Report) provides information for the Plutonium Isentropic Compression Experiment (Pu- ICE) program to support waste management and characterization efforts. Attachment 3-18 presents generator knowledge (GK) information specific to the eighteenth Pu-ICE conducted in August 2015, also known as ‘Shot 18 (Aug 2015) and Pu-ICE Z-2841 (1).’ Shot 18 (Aug 2015) was generated on August 28, 2015 (1). Calculations based on the isotopic content of Shot 18 (Aug 2015) and the measured mass of the containment system demonstrate the post-shot containment system is low-level waste (LLW). Therefore, this containment system will be managed at Sandia National Laboratory/New Mexico (SNL/NM) as LLW. Attachment 3-18 provides documentation of the TRU concentration and documents the concentration of any hazardous constituents.

  9. Using magnetization measurements to detect small amounts of plutonium hydride formation in plutonium metal

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jae Wook [Rutgers Univ., New Brunswick, NJ (United States); Mielke, Charles H. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Zapf, Vivien [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Baiardo, Joseph P. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Mitchell, Jeremy N. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Richmond, Scott [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Schwartz, Daniel S. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Mun, Eun D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Smith, Alice Iulia [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2014-10-20

    We report the formation of plutonium hydride in 2 at % Ga-stabilized δ-Pu, with 1 atomic % H charging. We show that magnetization measurements are a sensitive, quantitative measure of ferromagnetic plutonium hydride against the nonmagnetic background of plutonium. It was previously shown that at low hydrogen concentrations, hydrogen forms super-abundant vacancy complexes with plutonium, resulting in a bulk lattice contraction. Here we use magnetization, X-ray and neutron diffraction measurements to show that in addition to forming vacancy complexes, at least 30% of the H atoms bond with Pu to precipitate PuHx, largely on the surface of the sample with x ~ 1.9. We observe magnetic hysteresis loops below 40 K with magnetic remanence, consistent with precipitates of ferromagnetic PuH1.9.

  10. AMS of the Minor Plutonium Isotopes.

    Science.gov (United States)

    Steier, P; Hrnecek, E; Priller, A; Quinto, F; Srncik, M; Wallner, A; Wallner, G; Winkler, S

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure (239)Pu, (240)Pu, (241)Pu, (242)Pu and (244)Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of (244)Pu/(239)Pu = (5.7 ± 1.0) × 10(-5) based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the (242)Pu/(240)Pu ratio as an estimate of the initial (241)Pu/(239)Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method.

  11. Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids

    Science.gov (United States)

    Dalodière, Elodie; Virot, Matthieu; Morosini, Vincent; Chave, Tony; Dumas, Thomas; Hennig, Christoph; Wiss, Thierry; Dieste Blanco, Oliver; Shuh, David K.; Tyliszcak, Tolek; Venault, Laurent; Moisy, Philippe; Nikitenko, Sergey I.

    2017-03-01

    Fundamental knowledge on intrinsic plutonium colloids is important for the prediction of plutonium behaviour in the geosphere and in engineered systems. The first synthetic route to obtain salt-free intrinsic plutonium colloids by ultrasonic treatment of PuO2 suspensions in pure water is reported. Kinetics showed that both chemical and mechanical effects of ultrasound contribute to the mechanism of Pu colloid formation. In the first stage, fragmentation of initial PuO2 particles provides larger surface contact between cavitation bubbles and solids. Furthermore, hydrogen formed during sonochemical water splitting enables reduction of Pu(IV) to more soluble Pu(III), which then re-oxidizes yielding Pu(IV) colloid. A comparative study of nanostructured PuO2 and Pu colloids produced by sonochemical and hydrolytic methods, has been conducted using HRTEM, Pu LIII-edge XAS, and O K-edge NEXAFS/STXM. Characterization of Pu colloids revealed a correlation between the number of Pu-O and Pu-Pu contacts and the atomic surface-to-volume ratio of the PuO2 nanoparticles. NEXAFS indicated that oxygen state in hydrolytic Pu colloid is influenced by hydrolysed Pu(IV) species to a greater extent than in sonochemical PuO2 nanoparticles. In general, hydrolytic and sonochemical Pu colloids can be described as core-shell nanoparticles composed of quasi-stoichiometric PuO2 cores and hydrolyzed Pu(IV) moieties at the surface shell.

  12. Selecting a plutonium vitrification process

    Energy Technology Data Exchange (ETDEWEB)

    Jouan, A. [Centre d`Etudes de la Vallee du Rhone, Bagnols sur Ceze (France)

    1996-05-01

    Vitrification of plutonium is one means of mitigating its potential danger. This option is technically feasible, even if it is not the solution advocated in France. Two situations are possible, depending on whether or not the glass matrix also contains fission products; concentrations of up to 15% should be achievable for plutonium alone, whereas the upper limit is 3% in the presence of fission products. The French continuous vitrification process appears to be particularly suitable for plutonium vitrification: its capacity is compatible with the required throughout, and the compact dimensions of the process equipment prevent a criticality hazard. Preprocessing of plutonium metal, to convert it to PuO{sub 2} or to a nitric acid solution, may prove advantageous or even necessary depending on whether a dry or wet process is adopted. The process may involve a single step (vitrification of Pu or PuO{sub 2} mixed with glass frit) or may include a prior calcination step - notably if the plutonium is to be incorporated into a fission product glass. It is important to weigh the advantages and drawbacks of all the possible options in terms of feasibility, safety and cost-effectiveness.

  13. Plutonium Proliferation: The Achilles Heel of Disarmament

    Energy Technology Data Exchange (ETDEWEB)

    Leventhal, Paul (President, Nuclear Control Institute, Washington D.C.)

    2001-02-07

    Plutonium is a byproduct of nuclear fission, and it is produced at the rate of about 70 metric tons a year in the world's nuclear power reactors. Concerns about civilian plutonium ran high in the 1970s and prompted enactment of the Nuclear Non-Proliferation Act of 1978 to give the United States a veto over separating plutonium from U.S.-supplied uranium fuel. Over the years, however, so-called reactor-grade plutonium has become the orphan issue of nuclear non-proliferation, largely as a consequence of pressures from plutonium-separating countries. The demise of the fast breeder reactor and the reluctance of utilities to introduce plutonium fuel in light-water reactors have resulted in large surpluses of civilian, weapons-usable plutonium, which now approach in size the 250 tons of military plutonium in the world. Yet reprocessing of spent fuel for recovery and use of plutonium proceeds apace outside the United States and threatens to overwhelm safeguards and security measures for keeping this material out of the hands of nations and terrorists for weapons. A number of historical and current developments are reviewed to demonstrate that plutonium commerce is undercutting efforts both to stop the spread of nuclear weapons and to work toward eliminating existing nuclear arsenals. These developments include the breakdown of U.S. anti-plutonium policy, the production of nuclear weapons by India with Atoms-for-Peace plutonium, the U.S.-Russian plan to introduce excess military plutonium as fuel in civilian power reactors, the failure to include civilian plutonium and bomb-grade uranium in the proposed Fissile Material Cutoff Treaty, and the perception of emerging proliferation threats as the rationale for development of a ballistic missile defense system. Finally, immobilization of separated plutonium in high-level waste is explored as a proliferation-resistant and disarmament-friendly solution for eliminating excess stocks of civilian and military plutonium.

  14. Pu Anion Exchange Process Intensification

    Energy Technology Data Exchange (ETDEWEB)

    Taylor-Pashow, K. [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

    2015-10-08

    This project seeks to improve the efficiency of the plutonium anion-exchange process for purifying Pu through the development of alternate ion-exchange media. The objective of the project in FY15 was to develop and test a porous foam monolith material that could serve as a replacement for the current anion-exchange resin, Reillex® HPQ, used at the Savannah River Site (SRS) for purifying Pu. The new material provides advantages in efficiency over the current resin by the elimination of diffusive mass transport through large granular resin beads. By replacing the large resin beads with a porous foam there is much more efficient contact between the Pu solution and the anion-exchange sites present on the material. Several samples of a polystyrene based foam grafted with poly(4-vinylpyridine) were prepared and the Pu sorption was tested in batch contact tests.

  15. Examination of the effect of alpha radiolysis on plutonium(V) sorption to quartz using multiple plutonium isotopes.

    Science.gov (United States)

    Hixon, Amy E; Arai, Yuji; Powell, Brian A

    2013-08-01

    The objective of this research was to determine if radiolysis at the mineral surface was a plausible mechanism for surface-mediated reduction of plutonium. Batch sorption experiments were used to monitor the amount of plutonium sorbed to high-purity quartz as a function of time, pH, and total alpha radioactivity. Three systems were prepared using both (238)Pu and (242)Pu in order to increase the total alpha radioactivity of the mineral suspensions while maintaining a constant plutonium concentration. The fraction of sorbed plutonium increased with increasing time and pH regardless of the total alpha radioactivity of the system. Increasing the total alpha radioactivity of the solution had a negligible effect on the sorption rate. This indicated that surface-mediated reduction of Pu(V) in these systems was not due to radiolysis. Additionally, literature values for the Pu(V) disproportionation rate constant did not describe the experimental results. Therefore, Pu(V) disproportionation was also not a main driver for surface-mediated reduction of plutonium. Batch desorption experiments and X-ray absorption near edge structure spectroscopy were used to show that Pu(IV) was the dominant oxidation state of sorbed plutonium. Thus, it appears that the observed surface-mediated reduction of Pu(V) in the presence of high-purity quartz was based on the thermodynamic favorability of a Pu(IV) surface complex.

  16. National Low-Level Waste Management Program Radionuclide Report Series, Volume 17: Plutonium-239

    Energy Technology Data Exchange (ETDEWEB)

    J. P. Adams; M. L. Carboneau

    1999-03-01

    This report, Volume 17 of the National Low-Level Waste Management Program Radionuclide Report Series, discusses the radiological and chemical characteristics of plutonium-239 (Pu-239). This report also discusses waste types and forms in which Pu-239 can be found, waste and disposal information on Pu-239, and Pu-239 behavior in the environment and in the human body.

  17. Program Pu Futures 2006

    Energy Technology Data Exchange (ETDEWEB)

    Fluss, M

    2006-06-12

    The coordination chemistry of plutonium remains relatively unexplored. Thus, the fundamental coordination chemistry of plutonium is being studied using simple multi-dentate ligands with the intention that the information gleaned from these studies may be used in the future to develop plutonium-specific sequestering agents. Towards this goal, hard Lewis-base donors are used as model ligands. Maltol, an inexpensive natural product used in the commercial food industry, is an ideal ligand because it is an all-oxygen bidentate donor, has a rigid structure, and is of small enough size to impose little steric strain, allowing the coordination preferences of plutonium to be the deciding geometric factor. Additionally, maltol is the synthetic precursor of 3,4-HOPO, a siderophore-inspired bidentate moiety tested by us previously as a possible sequestering agent for plutonium under acidic conditions. As comparisons to the plutonium structure, Ce(IV) complexes of the same and related ligands were examined as well. Cerium(IV) complexes serve as good models for plutonium(IV) structures because Ce(IV) has the same ionic radius as Pu(IV) (0.94 {angstrom}). Plutonium(IV) maltol crystals were grown out of a methanol/water solution by slow evaporation to afford red crystals that were evaluated at the Advanced Light Source at Lawrence Berkeley National Laboratory using single crystal X-ray diffraction. Cerium(IV) complexes with maltol and bromomaltol were crystallized via slow evaporation of the mother liquor to afford tetragonal, black crystals. All three complexes crystallize in space group I4{sub 1}/a. The Ce(IV) complex is isostructural with the Pu(IV) complex, in which donating oxygens adopt a trigonal dodecahedral geometry around the metal with the maltol rings parallel to the crystallographic S{sub 4} axis and lying in a non-crystallographic mirror plane of D{sub 2d} molecular symmetry (Fig 1). The metal-oxygen bonds in both maltol complexes are equal to within 0.04 {angstrom

  18. Plutonium controversy

    Energy Technology Data Exchange (ETDEWEB)

    Richmond, C.R.

    1980-01-01

    The toxicity of plutonium is discussed, particularly in relation to controversies surrounding the setting of radiation protection standards. The sources, amounts of, and exposure pathways of plutonium are given and the public risk estimated. (ACR)

  19. Plutonium in Southern Hemisphere ocean Waters

    DEFF Research Database (Denmark)

    Hirose, K.; Aoyama, M.; Gastaud, J.

    2013-01-01

    Plutonium in seawater collected by the BEAGLE2003 cruise was determined using ICP- SF-MS and alpha spectrometry after Fe co-precipitation and radiochemical purification. Levels and distributions of dissolved plutonium activity concentrations in Southern Hemisphere ocean waters are summarized here......, including historical data. Pu-239 concentrations in surface water----of the central South Pacific (32.5 °S) in 2003 were around 1 mBq/m3. The 239Pu concentrations in the Indian Ocean surface waters (20°S) were similar to that in the South Pacific, whereas the 239Pu concentrations in the South Atlantic...... surface waters (30°S) were markedly lower than those in the South Pacific and Indian Oceans. The 239Pu vertical profile pattern was similar to that in the North Pacific subtropical gyre, although 239Pu concentrations in the deep South Pacific were significantly lower than those in the North Pacific. One...

  20. Experience gained with the Synroc demonstration plant at ANSTO and its relevance to plutonium immobilization

    Energy Technology Data Exchange (ETDEWEB)

    Jostsons, A.; Ridal, A.; Mercer, D.J.; Vance, E.R.L. [Australian Nuclear Science and Technology Organisation, Menai (Australia)

    1996-05-01

    The Synroc Demonstration Plant (SDP) was designed and constructed at Lucas Heights to demonstrate the feasibility of Synroc production on a commercial scale (10 kg/hr) with simulated Purex liquid HLW. Since commissioning of the SDP in 1987, over 6000 kg of Synroc has been fabricated with a range of feeds and waste loadings. The SDP utilises uniaxial hot-pressing to consolidate Synroc. Pressureless sintering and hot-isostatic pressing have also been studied at smaller scales. The results of this extensive process development have been incorporated in a conceptual design for a radioactive plant to condition HLW from a reprocessing plant with a capacity to treat 800 tpa of spent LWR fuel. Synroic containing TRU, including Pu, and fission products has been fabricated and characterised in a glove-box facility and hot cells, respectively. The extensive experience in processing of Synroc over the past 15 years is summarised and its relevance to immobilization of surplus plutonium is discussed.

  1. Plutonium immobilization plant using glass in existing facilities at the Savannah River Site

    Energy Technology Data Exchange (ETDEWEB)

    DiSabatino, A., LLNL

    1998-06-01

    The Plutonium Immobilization Plant (PIP) accepts plutonium (Pu) from pit conversion and from non-pit sources and, through a glass immobilization process, converts the plutonium into an immobilized form that can be disposed of in a high level waste (HLW) repository. The objective is to make an immobilized form, suitable for geologic disposal, in which the plutonium is as inherently unattractive and inaccessible as the plutonium in spent fuel from commercial reactors.

  2. Anthropogenic plutonium-244 in the environment: Insights into plutonium's longest-lived isotope.

    Science.gov (United States)

    Armstrong, Christopher R; Brant, Heather A; Nuessle, Patterson R; Hall, Gregory; Cadieux, James R

    2016-02-22

    Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., (244)Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic (244)Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken at SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Significant (244)Pu was measured in all of the years sampled with the highest amount observed in 2003. The (244)Pu content, in femtograms (fg = 10(-15) g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the (244)Pu/(239)Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively.

  3. Peculiar dynamical properties of plutonium hydrides

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    In the present work, the structure and spectra of PuH and PuH2 are defined by B3LYP/SDD method, from which the analytic potential energy function of PuH2 is derived. The analysis of quasi-classical molecular reaction dynamics is performed to study the state-state process of pu(7Fg) + H2(X1∑+g ). It is found that the reaction pu(7Fg) + H2(X1∑+g )→PuH2(X7B1) has no threshold. The simultaneous hydrogenation process of plutonium with the main product of PuH2 is theoretically proved for the first time.

  4. Probing Phonons in Plutonium

    Science.gov (United States)

    Wong, Joe

    2004-03-01

    The phonon spectra of plutonium and its alloys have been sought after in the past few decades following the discovery of this actinide element in 1941, but with no success. This was due to a combination of the high neutron absorption cross section of 239Pu, the common isotope, and non-availability of large single crystals of any Pu-bearing materials. We have recent designed a high resolution inelastic x-ray scattering experiment using a bright synchrotron x-ray beam at the European Sychrotron Radiation Facility (ESRF), Grenoble and mapped the full phonon dispersion curves of an fcc delta-phase polycrystalline Pu-Ga alloy (1). Several unusual features including, a large elastic anisotropy, a small shear elastic modulus C', a Kohn-like anomaly in the T1[011] branch, and a pronounced softening of the [111] transverse modes are found. These features can be related to the phase transitions of plutonium and to strong coupling between the lattice structure and the 5f valence instabilities. Our results also provide a critical test for theoretical treatments of highly correlated 5f electron systems as exemplified by recent dynamical mean field theory (DMFT) calculations for d-plutonium.(2) This work was performed in collaboration with Dr. M. Krisch (ESRF)) and Prof. T.-C. Chiang (UIU), and under the auspices of the U. S. Department of Energy by the University of California, Lawrence Livermore National Laboratory under Contract No. W-7405-Eng-48. 1. Joe Wong et al. Science, vol.301, 1078 (2003) 2. X. Dai et al. Science, vol.300, 953 (2003)

  5. Detecting low concentrations of plutonium hydride with magnetization measurements

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Jae Wook; Mun, E. D.; Baiardo, J. P.; Zapf, V. S.; Mielke, C. H. [National High Magnetic Field Laboratory, MPA-CMMS, Los Alamos National Laboratory (LANL), Los Alamos, New Mexico 87545 (United States); Smith, A. I.; Richmond, S.; Mitchell, J.; Schwartz, D. [Nuclear Material Science Group, MST-16, LANL, Los Alamos, New Mexico 87545 (United States)

    2015-02-07

    We report the formation of plutonium hydride in 2 at. % Ga-stabilized δ-Pu, with 1 at. % H charging. We show that magnetization measurements are a sensitive, quantitative measure of ferromagnetic plutonium hydride against the nonmagnetic background of plutonium. It was previously shown that at low hydrogen concentrations, hydrogen forms super-abundant vacancy complexes with plutonium, resulting in a bulk lattice contraction. Here, we use magnetization, X-ray, and neutron diffraction measurements to show that in addition to forming vacancy complexes, at least 30% of the H atoms bond with Pu to precipitate PuH{sub x} on the surface of the sample with x ∼ 1.9. We observe magnetic hysteresis loops below 40 K with magnetic remanence, consistent with ferromagnetic PuH{sub 1.9}.

  6. Plutonium stabilization and packaging system

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1996-05-01

    This document describes the functional design of the Plutonium Stabilization and Packaging System (Pu SPS). The objective of this system is to stabilize and package plutonium metals and oxides of greater than 50% wt, as well as other selected isotopes, in accordance with the requirements of the DOE standard for safe storage of these materials for 50 years. This system will support completion of stabilization and packaging campaigns of the inventory at a number of affected sites before the year 2002. The package will be standard for all sites and will provide a minimum of two uncontaminated, organics free confinement barriers for the packaged material.

  7. Liquid chromatographic studies on the behaviour of Pu(III), Pu(IV) and Pu(VI) on a RP stationary phase in presence of α-hydroxyisobutyric acid as a chelating agent

    Energy Technology Data Exchange (ETDEWEB)

    Jaison, P.G.; Kumar, Pranaw; Telmore, Vijay M. [Bhabha Atomic Research Centre, Mumbai (India). Fuel Chemistry Division

    2017-06-01

    Since plutonium possesses multiple oxidation states which can coexist in solution, a method for the identification of these oxidation states is important to understand its chemical processes. Liquid chromatographic studies were carried out to compare the chromatographic behaviour of different oxidation states of Pu in presence of the eluent, α-hydroxyisobutyric acid (HIBA). The three oxidation states of Pu viz. Pu(III), Pu(IV) and Pu(VI) were separated under optimised conditions. It was seen that the presence of the complexing agent influences the equilibrium of Pu(III)/(IV) as well as Pu(IV)/(VI) systems. Pu(III) to Pu(IV) conversion was found to be enhanced by high pH and concentration of HIBA whereas a relatively low pH and high concentration of HIBA promotes the conversion of Pu(VI) to Pu(IV).

  8. Preliminary safety evaluation for the plutonium stabilization and packaging system

    Energy Technology Data Exchange (ETDEWEB)

    Shapley, J.E., Fluor Daniel Hanford

    1997-03-14

    This Preliminary Safety Evaluation (PSE) describes and analyzes the installation and operation of the Plutonium Stabilization and Packaging System (SPS) at the Plutonium Finishing Plant (PFP). The SPS is a combination of components required to expedite the safe and timely storage of Plutonium (Pu) oxide. The SPS program will receive site Pu packages, process the Pu for storage, package the Pu into metallic containers, and safely store the containers in a specially modified storage vault. The location of the SPS will be in the 2736- ZB building and the storage vaults will be in the 2736-Z building of the PFP, as shown in Figure 1-1. The SPS will produce storage canisters that are larger than those currently used for Pu storage at the PFP. Therefore, the existing storage areas within the PFP secure vaults will require modification. Other modifications will be performed on the 2736-ZB building complex to facilitate the installation and operation of the SPS.

  9. Effect of compositional variation in plutonium on process shielding design

    Energy Technology Data Exchange (ETDEWEB)

    Brown, T.H.

    1997-11-01

    Radiation dose rate from plutonium with high {sup 239}Pu content varies with initial nuclidic content, radioactive decay time, and impurity elemental content. The two idealized states of old plutonium and clean plutonium, whose initial compositions are given, provide approximate upper and lower bounds on dose rate variation. Whole-body dose rates were calculated for the two composition states, using unshielded and shielded plutonium spheres of varying density. The dose rates from these variable density spheres are similar to those from expanded plutonium configurations encountered during processing. The dose location of 40 cm from the sphere center is representative of operator standoff for direct handling of plutonium inside a glove box. The results have shielding implications for glove boxes with only structurally inherent shielding, especially for processing of old plutonium in an expanded configuration. Further reduction in total dose rate by using lead to reduce photon dose rate is shown for two density cases representing compact and expanded plutonium configurations.

  10. Plutonium Metallurgy

    Energy Technology Data Exchange (ETDEWEB)

    Freibert, Franz J. [Los Alamos National Laboratory

    2012-08-09

    Due to its nuclear properties, Pu will remain a material of global interest well into the future. Processing, Structure, Properties and Performance remains a good framework for discussion of Pu materials science Self-irradiation and aging effects continue to be central in discussions of Pu metallurgy Pu in its elemental form is extremely unstable, but alloying helps to stabilize Pu; but, questions remain as to how and why this stabilization occurs. Which is true Pu-Ga binary phase diagram: US or Russian? Metallurgical issues such as solute coring, phase instability, crystallographic texture, etc. result in challenges to casting, processing, and properties modeling and experiments. For Ga alloyed FCC stabilized Pu, temperature and pressure remain as variables impacting phase stability.

  11. Concentration and purification of plutonium or thorium

    Science.gov (United States)

    Hayden, John A.; Plock, Carl E.

    1976-01-01

    In this invention a first solution obtained from such as a plutonium/thorium purification process or the like, containing plutonium (Pu) and/or thorium (Th) in such as a low nitric acid (HNO.sub.3) concentration may have the Pu and/or Th separated and concentrated by passing an electrical current from a first solution having disposed therein an anode to a second solution having disposed therein a cathode and separated from the first solution by a cation permeable membrane, the Pu or Th cation permeating the cation membrane and forming an anionic complex within the second solution, and electrical current passage affecting the complex formed to permeate an anion membrane separating the second solution from an adjoining third solution containing disposed therein an anode, thereby effecting separation and concentration of the Pu and/or Th in the third solution.

  12. Iron Corrosion Observations: Pu(VI)-Fe Reduction Studies

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Donald T. [Los Alamos National Laboratory; Swanson, Juliet S. [Los Alamos National Laboratory; Richmann, Michael K. [Los Alamos National Laboratory; Lucchini, Jean-Francois [Los Alamos National Laboratory; Borkowski, Marian [Los Alamos National Laboratory

    2012-09-11

    Iron and Pu Reduction: (1) Very different appearances in iron reaction products were noted depending on pH, brine and initial iron phase; (2) Plutonium was associated with the Fe phases; (3) Green rust was often noted at the higher pH; (4) XANES established the green rust to be an Fe2/3 phase with a bromide center; and (5) This green rust phase was linked to Pu as Pu(IV).

  13. Design-Only Conceptual Design Report: Plutonium Immobilization Plant

    Energy Technology Data Exchange (ETDEWEB)

    DiSabatino, A.; Loftus, D.

    1999-01-01

    This design-only conceptual design report was prepared to support a funding request by the Department of Energy Office of Fissile Materials Disposition for engineering and design of the Plutonium Immobilization Plant, which will be used to immobilize up to 50 tonnes of surplus plutonium. The siting for the Plutonium Immobilization Plant will be determined pursuant to the site-specific Surplus Plutonium Disposition Environmental Impact Statement in a Plutonium Deposition Record of Decision in early 1999. This document reflects a new facility using the preferred technology (ceramic immobilization using the can-in-canister approach) and the preferred site (at Savannah River). The Plutonium Immobilization Plant accepts plutonium from pit conversion and from non-pit sources and, through a ceramic immobilization process, converts the plutonium into mineral-like forms that are subsequently encapsulated within a large canister of high-level waste glass. The final immobilized product must make the plutonium as inherently unattractive and inaccessible for use in nuclear weapons as the plutonium in spent fuel from commercial reactors and must be suitable for geologic disposal. Plutonium immobilization at the Savannah River Site uses: (1) A new building, the Plutonium Immobilization Plant, which will convert non-pit surplus plutonium to an oxide form suitable for the immobilization process, immobilize plutonium in a titanate-based ceramic form, place cans of the plutonium-ceramic forms into magazines, and load the magazines into a canister; (2) The existing Defense Waste Processing Facility for the pouring of high-level waste glass into the canisters; and (3) The Actinide Packaging and Storage Facility to receive and store feed materials. The Plutonium Immobilization Plant uses existing Savannah River Site infra-structure for analytical laboratory services, waste handling, fire protection, training, and other support utilities and services. The Plutonium Immobilization Plant

  14. An analysis of plutonium immobilization versus the "spent fuel" standard

    Energy Technology Data Exchange (ETDEWEB)

    Gray, W L; McKibben, J M

    1998-06-16

    Safe Pu management is an important and urgent task with profound environmental, national, and international security implications. Presidential Policy Directive 13 and analyses by scientific, technical, and international policy organizations brought about a focused effort within the Department of Energy (DOE) to identify and implement long-term disposition paths for surplus Pu. The principal goal is to render surplus Pu as inaccessible and unattractive for reuse in nuclear weapons as Pu in spent reactor fuel. In the Programmatic Environmental Impact Statement and Record of Decision for the Storage and Disposition of Weapons- Usable Fissile Materials (1997), DOE announced pursuit of two disposition technologies: (1) irradiation of Pu as MOX fuel in existing reactors and (2) immobilization of Pu into solid forms containing fission products as a radiation barrier. DOE chose an immobilization approach that includes "use of the can-in-canister option.. . for a portion of the surplus, non-pit Pu material." In the can-in-canister approach, cans of glass or ceramic forms containing Pu are encapsulated within canisters of HLW glass. In support of the selection process, a technical evaluation of retrievability and recoverability of Pu from glass and ceramic forms by a host nation and by rogue nations or subnational groups was completed. The evaluation involved determining processes and flowsheets for Pu recovery, comparing these processes against criteria and metrics established by the Fissile Materials Disposition Program and then comparing the recovery processes against each other and against SNF processes.

  15. Preparation of Pu Target with Small Area

    Institute of Scientific and Technical Information of China (English)

    SUN; Xiao-yi; MAO; Guo-shu; HUANG; Kun; YANG; Lei; YANG; Su-liang; YANG; Chun-li; SUN; Hong-qing; MA; Peng

    2015-01-01

    Plutonium can be electrodeposited in ammonium oxalate,ammonium sulfate and ammonium chloride systems,but there is white layer appeared when the diameter of the active area is7mm and Pu is electrodeposited in isopropanol,and large amount of hydrogen is generated near the cathode in ammonium sulfate,which covers

  16. Vertical distribution of (241)Pu in the southern Baltic Sea sediments.

    Science.gov (United States)

    Strumińska-Parulska, Dagmara I

    2014-12-15

    The vertical distribution of plutonium (241)Pu in marine sediments can assist in determining the deposition history and sedimentation process of analyzed regions. In addition, (241)Pu/(239+240)Pu activity ratio could be used as a sensitive fingerprint for radioactive source identification. The present preliminary studies on vertical distribution of (241)Pu in sediments from four regions of the southern Baltic Sea are presented. The distribution of (241)Pu was not uniform and depended on sediment geomorphology and depth as well as location. The highest concentrations of plutonium were found in the surface layers of all analyzed sediments and originated from the Chernobyl accident.

  17. Plutonium transport in the environment.

    Science.gov (United States)

    Kersting, Annie B

    2013-04-01

    The recent estimated global stockpile of separated plutonium (Pu) worldwide is about 500 t, with equal contributions from nuclear weapons and civilian nuclear energy. Independent of the United States' future nuclear energy policy, the current large and increasing stockpile of Pu needs to be safely isolated from the biosphere and stored for thousands of years. Recent laboratory and field studies have demonstrated the ability of colloids (1-1000 nm particles) to facilitate the migration of strongly sorbing contaminants such as Pu. In understanding the dominant processes that may facilitate the transport of Pu, the initial source chemistry and groundwater chemistry are important factors, as no one process can explain all the different field observations of Pu transport. Very little is known about the molecular-scale geochemical and biochemical mechanisms controlling Pu transport, leaving our conceptual model incomplete. Equally uncertain are the conditions that inhibit the cycling and mobility of Pu in the subsurface. Without a better mechanistic understanding for Pu at the molecular level, we cannot advance our ability to model its transport behavior and achieve confidence in predicting long-term transport. Without a conceptual model that can successfully predict long-term Pu behavior and ultimately isolation from the biosphere, the public will remain skeptical that nuclear energy is a viable and an attractive alternative to counter global warming effects of carbon-based energy alternatives. This review summarizes our current understanding of the relevant conditions and processes controlling the behavior of Pu in the environment, gaps in our scientific knowledge, and future research needs.

  18. Ultra-small plutonium oxide nanocrystals: an innovative material in plutonium science.

    Science.gov (United States)

    Hudry, Damien; Apostolidis, Christos; Walter, Olaf; Janssen, Arne; Manara, Dario; Griveau, Jean-Christophe; Colineau, Eric; Vitova, Tonya; Prüssmann, Tim; Wang, Di; Kübel, Christian; Meyer, Daniel

    2014-08-11

    Apart from its technological importance, plutonium (Pu) is also one of the most intriguing elements because of its non-conventional physical properties and fascinating chemistry. Those fundamental aspects are particularly interesting when dealing with the challenging study of plutonium-based nanomaterials. Here we show that ultra-small (3.2±0.9 nm) and highly crystalline plutonium oxide (PuO2 ) nanocrystals (NCs) can be synthesized by the thermal decomposition of plutonyl nitrate ([PuO2 (NO3 )2 ]⋅3 H2 O) in a highly coordinating organic medium. This is the first example reporting on the preparation of significant quantities (several tens of milligrams) of PuO2 NCs, in a controllable and reproducible manner. The structure and magnetic properties of PuO2 NCs have been characterized by a wide variety of techniques (powder X-ray diffraction (PXRD), X-ray absorption fine structure (XAFS), X-ray absorption near edge structure (XANES), TEM, IR, Raman, UV/Vis spectroscopies, and superconducting quantum interference device (SQUID) magnetometry). The current PuO2 NCs constitute an innovative material for the study of challenging problems as diverse as the transport behavior of plutonium in the environment or size and shape effects on the physics of transuranium elements.

  19. LWR spent fuel reduction by the removal of U and the compact storage of Pu with FP for long-term nuclear sustainability

    Energy Technology Data Exchange (ETDEWEB)

    Fukasawa, T.; Hoshino, K. [Hitachi-GE Nuclear Energy, Ltd, 3-1-1 Saiwai, Hitachi, Ibaraki, 317-0073 (Japan); Takano, M. [Japan Atomic Energy Agency, 3-1-1 Saiwai, Hitachi, Ibaraki, 317-0073 (Japan); Sato, S. [Hokkaido University, 3-1-1 Saiwai, Hitachi, Ibaraki, 317-0073 (Japan); Shimazu, Y. [Fukui University, 3-1-1 Saiwai, Hitachi, Ibaraki, 317-0073 (Japan)

    2013-07-01

    Fast breeder reactors (FBR) nuclear fuel cycle is needed for long-term nuclear sustainability while preventing global warming and maximum utilizing the limited uranium (U) resources. The 'Framework for Nuclear Energy Policy' by the Japanese government on October 2005 stated that commercial FBR deployment will start around 2050 under its suitable conditions by the successive replacement of light water reactors (LWR) to FBR. Even after Fukushima Daiichi Nuclear Power Plant accident which made Japanese tendency slow down the nuclear power generation activities, Japan should have various options for energy resources including nuclear, and also consider the delay of FBR deployment and increase of LWR spent fuel (LWR-SF) storage amounts. As plutonium (Pu) for FBR deployment will be supplied from LWR-SF reprocessing and Japan will not possess surplus Pu, the authors have developed the flexible fuel cycle initiative (FFCI) for the transition from LWR to FBR. The FFCI system is based on the possibility to stored recycled materials (U, Pu)temporarily for a suitable period according to the FBR deployment rate to control the Pu demand/supply balance. This FFCI system is also effective after the Fukushima accident for the reduction of LWR-SF and future LWR-to-FBR transition. (authors)

  20. Plutonium worker dosimetry.

    Science.gov (United States)

    Birchall, Alan; Puncher, M; Harrison, J; Riddell, A; Bailey, M R; Khokryakov, V; Romanov, S

    2010-05-01

    Epidemiological studies of the relationship between risk and internal exposure to plutonium are clearly reliant on the dose estimates used. The International Commission on Radiological Protection (ICRP) is currently reviewing the latest scientific information available on biokinetic models and dosimetry, and it is likely that a number of changes to the existing models will be recommended. The effect of certain changes, particularly to the ICRP model of the respiratory tract, has been investigated for inhaled forms of (239)Pu and uncertainties have also been assessed. Notable effects of possible changes to respiratory tract model assumptions are (1) a reduction in the absorbed dose to target cells in the airways, if changes under consideration are made to the slow clearing fraction and (2) a doubling of absorbed dose to the alveolar region for insoluble forms, if evidence of longer retention times is taken into account. An important factor influencing doses for moderately soluble forms of (239)Pu is the extent of binding of dissolved plutonium to lung tissues and assumptions regarding the extent of binding in the airways. Uncertainty analyses have been performed with prior distributions chosen for application in epidemiological studies. The resulting distributions for dose per unit intake were lognormal with geometric standard deviations of 2.3 and 2.6 for nitrates and oxides, respectively. The wide ranges were due largely to consideration of results for a range of experimental data for the solubility of different forms of nitrate and oxides. The medians of these distributions were a factor of three times higher than calculated using current default ICRP parameter values. For nitrates, this was due to the assumption of a bound fraction, and for oxides due mainly to the assumption of slower alveolar clearance. This study highlights areas where more research is needed to reduce biokinetic uncertainties, including more accurate determination of particle transport rates

  1. PLUTONIUM LOADING CAPACITY OF REILLEX HPQ ANION EXCHANGE COLUMN - AFS-2 PLUTONIUM FLOWSHEET FOR MOX

    Energy Technology Data Exchange (ETDEWEB)

    Kyser, E.; King, W.; O' Rourke, P.

    2012-07-26

    Radioactive plutonium (Pu) anion exchange column experiments using scaled HB-Line designs were performed to investigate the dependence of column loading performance on the feed composition in the H-Canyon dissolution process for plutonium oxide (PuO{sub 2}) product shipped to the Mixed Oxide (MOX) Fuel Fabrication Facility (MFFF). These loading experiments show that a representative feed solution containing {approx}5 g Pu/L can be loaded onto Reillex{trademark} HPQ resin from solutions containing 8 M total nitrate and 0.1 M KF provided that the F is complexed with Al to an [Al]/[F] molar ratio range of 1.5-2.0. Lower concentrations of total nitrate and [Al]/[F] molar ratios may still have acceptable performance but were not tested in this study. Loading and washing Pu losses should be relatively low (<1%) for resin loading of up to 60 g Pu/L. Loading above 60 g Pu/L resin is possible, but Pu wash losses will increase such that 10-20% of the additional Pu fed may not be retained by the resin as the resin loading approaches 80 g Pu/L resin.

  2. Magnetism, superconductivity and Fermi surfaces of plutonium compounds

    Energy Technology Data Exchange (ETDEWEB)

    Haga, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan)]. E-mail: haga.yoshinori@jaea.go.jp; Aoki, D. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Yamagami, H. [Department of Physics, Faculty of Science, Kyoto Sangyo University, Kyoto 603-8555 (Japan); Matsuda, T.D. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Nakajima, K. [Nuclear Science and Engineering Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Arai, Y. [Nuclear Science and Engineering Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Homma, Y. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Shiokawa, Y. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Yamamoto, E. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Nakamura, A. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Onuki, Y. [Graduate School of Science, Osaka University, Toyonaka, Osaka 560-0043 (Japan); Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan)

    2007-03-15

    Single crystals of plutonium compounds PuRhGa{sub 5} and PuIn{sub 3} are successfully grown. For PuRhGa{sub 5}, anisotropy of the superconducting upper critical field was found and analyzed by the anisotropic mass model, consistent with quasi-two-dimensional electronic states predicted by band calculations. On the other hand, the de Haas-van Alphen oscillation was observed in PuIn{sub 3}. By comparing with the band calculations, it is concluded that 5f electrons are itinerant in PuIn{sub 3}.

  3. Development of first ever scanning probe microscopy capabilities for plutonium

    Science.gov (United States)

    Beaux, Miles F.; Cordoba, Miguel Santiago; Zocco, Adam T.; Vodnik, Douglas R.; Ramos, Michael; Richmond, Scott; Moore, David P.; Venhaus, Thomas J.; Joyce, Stephen A.; Usov, Igor O.

    2017-04-01

    Scanning probe microscopy capabilities have been developed for plutonium and its derivative compounds. Specifically, a scanning tunneling microscope and an atomic force microscope housed in an ultra-high vacuum system and an inert atmosphere glove box, respectively, were prepared for the introduction of small non-dispersible δ-Pu coupons. Experimental details, procedures, and preliminary imaging of δ-Pu coupons are presented to demonstrate the functionality of these new capabilities. These first of a kind capabilities for plutonium represent a significant step forward in the ability to characterize and understand plutonium surfaces with high spatial resolution.

  4. Speciation and interactions of plutonium with humic substances and kaolinite in aquifer systems

    Energy Technology Data Exchange (ETDEWEB)

    Banik, N.L. [Institut fuer Kernchemie, Johannes Gutenberg-Universitaet, D-55099 Mainz (Germany)], E-mail: banik@uni-mainz.de; Buda, R.A. [Institut fuer Kernchemie, Johannes Gutenberg-Universitaet, D-55099 Mainz (Germany); Buerger, S. [Oak Ridge National Laboratory, Chemical and Isotope Mass Spectrometry Group, Transuranium Research Institute, Oak Ridge TN 37831 (United States); Kratz, J.V. [Institut fuer Kernchemie, Johannes Gutenberg-Universitaet, D-55099 Mainz (Germany)], E-mail: JVKratz@uni-mainz.de; Trautmann, N. [Institut fuer Kernchemie, Johannes Gutenberg-Universitaet, D-55099 Mainz (Germany)

    2007-10-11

    The speciation of plutonium (Pu) in contact with humic substances (HS) and kaolinite has been performed in aquifer systems. Mainly the redox behavior, complexation, and sorption of plutonium are discussed here. The redox behavior of Pu(VI) in contact with HS was studied and it was found that Pu(VI) is reduced to Pu(III) and Pu(IV) within a couple of weeks. The complexation constants (log {beta}{sub LC}) of Pu(III) and Pu(IV) with HS have been determined by means of the ultrafiltration method. Furthermore, the sorption of Pu(III) and Pu(IV) onto kaolinite has been investigated as a function of pH by batch experiments under aerobic and anaerobic conditions.

  5. SEPARATION OF NEPTUNIUM FROM PLUTONIUM BY CHLORINATION AND SUBLIMATION

    Science.gov (United States)

    Fried, S.M.

    1958-11-18

    A process is described for separating neptunium from plutonium. The method consists in chlorinating a mixture of the oxides of Np and Pu by contacting the mixture with carbon tetrachloride at about 500 icient laborato C. ln this manner the Np is converted to the tetrachlorlde and the Pu converted to the trichloride. Since NpCl/sub 4/ is more latile than PuCl/sub 3/, the separation ls effected by vaporing sad subsequently condenslng the NpCl/sub 4/.

  6. Chemical thermodynamics of nuclear materials. 6. (Plutonium + hydrogen)

    Energy Technology Data Exchange (ETDEWEB)

    Smith, C.M.; Hodges, A.E. III; Haschke, J.M.; Oetting, F.L. (Rockwell International Corp., Golden, CO (USA). Rocky Flats Plant)

    1982-02-01

    The standard enthalpies of formation of cubic PuHsub(x)(c), where x = 1.99, 2.21, and 2.62, were determined by solution calorimetry and the results are reported. The results are in reasonable agreement with the enthalpies obtained by Gibbs-Duhem integration of the equilibrium hydrogen pressure for (plutonium + hydrogen) over the composition range PuHsub(1.9) to PuHsub(3.0).

  7. Ultra-sensitive detection of plutonium by accelerator mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Fifield, L.K.; Cresswell, R.G.; Ophel, T.R.; Ditada, M. [Australian National Univ., Canberra, ACT (Australia). Dept. of Nuclear Physics; Day, J.P.; Clacher, A. [Manchester Univ. (United Kingdom). Dept. of Chemistry; Priest, N.D. [AEA Technology, Harwell (United Kingdom)

    1996-12-31

    On the bases of the measurements performed to date, a sensitivity of 10{sup 6} atoms is achievable with accelerator mass spectroscopy (AMS) for each of the plutonium isotopes. Not only does this open the way to the sort of study outlined, but it also makes possible other novel applications, of which two examples are given: (i)the ration of {sup 240}Pu to {sup 239}Pu as a sensitive indicator of the source of the plutonium; (ii) the biochemistry of plutonium in humans. The ultra-sensitive atom counting capability of AMS will make it possible to use the very long-lived {sup 244}Pu (8x10{sup 7}a) in human volunteer studies without any significant increase in radiation body burden. This paper will describe the AMS technique as applied to plutonium using the ANU`s 14UD accelerator, will present the results obtained to date, and will discuss the prospects for the future.

  8. Effect of microorganisms on the plutonium oxidation states

    Energy Technology Data Exchange (ETDEWEB)

    Luksiene, Benedikta, E-mail: bena@ar.fi.lt [Center for Physical Sciences and Technology, Savanoriu ave 231, LT-02300 Vilnius (Lithuania); Druteikiene, Ruta [Center for Physical Sciences and Technology, Savanoriu ave 231, LT-02300 Vilnius (Lithuania); Peciulyte, Dalia [Nature Research Centre, Akademijos street 2, LT-08412 Vilnius (Lithuania); Baltrunas, Dalis; Remeikis, Vidmantas [Center for Physical Sciences and Technology, Savanoriu ave 231, LT-02300 Vilnius (Lithuania); Paskevicius, Algimantas [Nature Research Centre, Akademijos street 2, LT-08412 Vilnius (Lithuania)

    2012-03-15

    Particular microbes from substrates at the low-level radioactive waste repository in the Ignalina NPP territory were exposed to {sup 239}Pu (IV) at low pH under aerobic conditions. Pu(III) and Pu(IV) were separated and quantitatively evaluated using the modified anion exchange method and alpha spectrometry. Tested bacteria Bacillus mycoides and Serratia marcescens were more effective in Pu reduction than Rhodococcus fascians. Fungi Paecillomyces lilacinus and Absidia spinosa var. spinosa as well as bacterium Rhodococcus fascians did not alter the plutonium oxidation state. - Highlights: Black-Right-Pointing-Pointer Particular microbes from low-level radioactive waste repository were exposed to Pu (IV). Black-Right-Pointing-Pointer Some tested bacteria induced slight Pu (IV) reduction at low pH under aerobic conditions. Black-Right-Pointing-Pointer Tested fungi did not show peculiarities to alter Pu oxidation state. Black-Right-Pointing-Pointer The modified radiochemical method was applied to differentiate Pu oxidation states.

  9. Surplus Value & Income Distribution

    OpenAIRE

    Yoshizawa,Masayasu

    1993-01-01

    Introduction 1. Marx's Theory of Surplus-Value 1.1. Use-Value and Exchange-Value 1.2. Surplus-Value 1.3. Variable Capital and Constant Capital 2. Implications of Marx's Theory of Surplus-Value 2.1. First Implication-Exploitation 2.2. Second Implication-Deviation of Price from Value 2.3. Third Implication-Capitalist Corporation 3. Capital Accumulation and Income Distribution 3.1. The Effect of Capital Accumulation 3.2. Fall in the Rate of Profit 4. Conclusion 

  10. High-Resolution Inductively Coupled Plasma Optical Emission Spectrometry for (234)U/(238)Pu Age Dating of Plutonium Materials and Comparison to Sector Field Inductively Coupled Plasma Mass Spectrometry.

    Science.gov (United States)

    Krachler, Michael; Alvarez-Sarandes, Rafael; Rasmussen, Gert

    2016-09-06

    Employing a commercial high-resolution inductively coupled plasma optical emission spectrometry (HR-ICP-OES) instrument, an innovative analytical procedure for the accurate determination of the production age of various Pu materials (Pu powder, cardiac pacemaker battery, (242)Cm heat source, etc.) was developed and validated. This undertaking was based on the fact that the α decay of (238)Pu present in the investigated samples produced (234)U and both mother and daughter could be identified unequivocally using HR-ICP-OES. Benefiting from the high spectral resolution of the instrument (U and (238)Pu were selectively and directly determined in the dissolved samples, i.e., without a chemical separation of the two analytes from each other. Exact emission wavelengths as well as emission spectra of (234)U centered around λ = 411.590 nm and λ = 424.408 nm are reported here for the first time. Emission spectra of the isotopic standard reference material IRMM-199, comprising about one-third each of (233)U, (235)U, and (238)U, confirmed the presence of (234)U in the investigated samples. For the assessment of the (234)U/(238)Pu amount ratio, the emission signals of (234)U and (238)Pu were quantified at λ = 424.408 nm and λ = 402.148 nm, respectively. The age of the investigated samples (range: 26.7-44.4 years) was subsequently calculated using the (234)U/(238)Pu chronometer. HR-ICP-OES results were crossed-validated through sector field inductively coupled plasma mass spectrometry (SF-ICPMS) analysis of the (234)U/(238)Pu amount ratio of all samples applying isotope dilution combined with chromatographic separation of U and Pu. Available information on the assumed ages of the analyzed samples was consistent with the ages obtained via the HR-ICP-OES approach. Being based on a different physical detection principle, HR-ICP-OES provides an alternative strategy to the well-established mass spectrometric approach and thus effectively adds to the quality assurance of (234)U

  11. Measurement and interpretation of plutonium spectra

    Energy Technology Data Exchange (ETDEWEB)

    Blaise, J.; Fred, M.S.; Carnall, W.T.; Crosswhite, H.M.; Crosswhite, H.

    1982-01-01

    The atomic spectroscopic data available for plutonium are among the rickest of any in the periodic system. They include high-resolution grating and Fourier-transform spectra as well as extensive Zeeman and isotope-shift studies. We summarize the present status of the term analysis and cite the configurations that have been identified. A least-squares adjustment of a parametric Hamiltonian for configurations of both Pu I and Pu II has shown that almost all of the expected low levels are now known. The use of a model Hamiltonian applicable to both lanthanide and actinide atomic species has been applied to the low configurations of Pu I and Pu II making use of trends predicted by ab initio calculations. This same model has been used to describe the energy levels of Pu/sup 3 +/ in LaCl/sub 3/, and an extension has permitted preliminary calculations of the spectra of other valence states.

  12. Study on Analytical Method of Pu(Ⅲ, Ⅳ) and U(Ⅳ) in 1BP

    Institute of Scientific and Technical Information of China (English)

    LIU; Huan-liang; ZHANG; Li-hua; FAN; De-jun; WANG; Ling; QIAN; Hong-juan

    2013-01-01

    U(Ⅳ)is taken as reductant in uranium and plutonium separation process of China spent nuclear fuel reprocessing pilot plant.Rapid determining the concentrations of Pu(Ⅲ)/Pu(Ⅳ)and U(Ⅳ)in 1BP is vital to monitor 1B processing stage and condition the subsequent processing solution.A rapid method for determining the concentrations of Pu(Ⅲ)/Pu(Ⅳ)and U(Ⅳ)in 1BP was developed

  13. Adsorption behaviour of PuF6 on UO2F2 by the use of 236Pu

    Science.gov (United States)

    Sato, Nobuaki; Matsuda, Minoru; Mitsugashira, Toshiaki; Kirishima, Akira

    2010-03-01

    To know the behavior of plutonium in the fluoride volatility process (FLUOREX PROCESS) for the spent nuclear fuel, both UO2 and PuO2 are fluorinated by fluorine forming volatile UF6 and PuF6, respectively. Then PuF6 is separated and recovered from UF6 by using adsorption materials such as uranyl fluoride UO2F2. In this paper, adsorption behavior of PuF6on UO2F2 was examined by the use of 236Pu tracer. First, the stability of UO2F2 in F2atmosphere was analyzed by TG-DTA method showing that uranium volatilized completely over 350 °C by the formation of UF6 and the adsorption of plutonium by UO2F2 should be done at temperatures lower than 250 °C. The behavior of PtF6 as a chemical analogue of PuF6 was also conducted for comparison and it showed that the deposition of PtF4 on UO2F2 at 200 °C. When the 236Pu doped U3O8 was reacted with 10%F2-He gas, the PuF6 vaporized at ca. 600 °C. Then adsorption of 236Pu on UO2F2 was observed by α ray measurement. The adsorption mechanism of Pu on UO2F2 was discussed with experimental data and thermodynamic consideration.

  14. Determination of plutonium isotopes in seawater reference materials using isotope-dilution ICP-MS.

    Science.gov (United States)

    Zheng, Jian; Yamada, Masatoshi

    2012-09-01

    We analyzed the activities of (239)Pu, (240)Pu, (239+240)Pu, (241)Pu, the ratio of number of atoms (atom ratio) for (240)Pu/(239)Pu, and the activity ratio of (241)Pu/(239+240)Pu in seawater reference materials, IAEA-443 and IAEA-381, using a highly sensitive isotope dilution sector field inductively coupled plasma mass spectrometry method. With a mean chemical yield of 65% determined with (242)Pu as a tracer, we found that the experimentally established values in IAEA-443 for (239)Pu, (240)Pu, (241)Pu and (239+240)Pu activities are almost the same as those in IAEA-381. Regarding the (239+240)Pu activity, we provided the most precise and accurate result among the twelve laboratories, which participated in the interlaboratory comparison. In addition, for the (240)Pu/(239)Pu atom ratio, our results for IAEA-381 (0.2315±0.0008) and IAEA-443 (0.2325±0.0008) are in good agreement with the IAEA information value (0.229±0.006), but have much smaller uncertainty. Since the new seawater reference material, IAEA-443, is commercially available, it can be used not only for method validation for seawater plutonium isotope ratio and activity analysis, but also for more general use as a plutonium isotope standard for mass discrimination correction for other environmental samples.

  15. Benefits of a Surplus

    Institute of Scientific and Technical Information of China (English)

    2006-01-01

    China has growing surplus in its trade and capital accounts, which have prompted warnings and criticism from both domestic and foreign economists. Some think this represents an imbalance in international payments and suggest China speed up the appreciation of the yuan to adjust that imbalance. But Qu Hongbin, Chief China Economist for HSBC, and Ma Xiaoping, an economic analyst, argue that the double-surplus issue should be viewed from a broader perspective. In their article in The Economic Observer, they...

  16. Stabilization of plutonium nano-colloids by epitaxial distortion on mineral surfaces.

    Science.gov (United States)

    Powell, Brian A; Dai, Zurong; Zavarin, Mavrik; Zhao, Pihong; Kersting, Annie B

    2011-04-01

    The subsurface migration of Pu may be enhanced by the presence of colloidal forms of Pu. Therefore, complete evaluation of the risk posed by subsurface Pu contamination needs to include a detailed physical/chemical understanding of Pu colloid formation and interactions of Pu colloids with environmentally relevant solid phases. Transmission electron microscopy (TEM) was used to characterize Pu nanocolloids and interactions of Pu nanocolloids with goethite and quartz. We report that intrinsic Pu nanocolloids generated in the absence of goethite or quartz were 2-5 nm in diameter, and both electron diffraction analysis and HRTEM confirm the expected Fm3m space group with the fcc, PuO2 structure. Plutonium nanocolloids formed on goethite have undergone a lattice distortion relative to the ideal fluorite-type structure, fcc, PuO2, resulting in the formation of a bcc, Pu4O7 structure. This structural distortion results from an epitaxial growth of the plutonium colloid on goethite, leading to stronger binding of plutonium to goethite compared with other minerals such as quartz, where the distortion was not observed. This finding provides new insight for understanding how molecular-scale behavior at the mineral-water interface may facilitate transport of plutonium at the field scale.

  17. Plutonium Immobilization Project System Design Description for Can Loading System

    Energy Technology Data Exchange (ETDEWEB)

    Kriikku, E.

    2001-02-15

    The purpose of this System Design Description (SDD) is to specify the system and component functions and requirements for the Can Loading System and provide a complete description of the system (design features, boundaries, and interfaces), principles of operation (including upsets and recovery), and the system maintenance approach. The Plutonium Immobilization Project (PIP) will immobilize up to 13 metric tons (MT) of U.S. surplus weapons usable plutonium materials.

  18. Conceptual Design for the Pilot-Scale Plutonium Oxide Processing Unit in the Radiochemical Processing Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J.; Meier, David E.; Tingey, Joel M.; Casella, Amanda J.; Delegard, Calvin H.; Edwards, Matthew K.; Jones, Susan A.; Rapko, Brian M.

    2014-08-05

    This report describes a conceptual design for a pilot-scale capability to produce plutonium oxide for use as exercise and reference materials, and for use in identifying and validating nuclear forensics signatures associated with plutonium production. This capability is referred to as the Pilot-scale Plutonium oxide Processing Unit (P3U), and it will be located in the Radiochemical Processing Laboratory at the Pacific Northwest National Laboratory. The key unit operations are described, including plutonium dioxide (PuO2) dissolution, purification of the Pu by ion exchange, precipitation, and conversion to oxide by calcination.

  19. Zone refining of plutonium metal

    Energy Technology Data Exchange (ETDEWEB)

    Blau, Michael S. [Univ. of Idaho, Moscow, ID (United States)

    1994-08-01

    The zone refining process was applied to Pu metal containing known amounts of impurities. Rod specimens of plutonium metal were melted into and contained in tantalum boats, each of which was passed horizontally through a three-turn, high-frequency coil in such a manner as to cause a narrow molten zone to pass through the Pu metal rod 10 times. The impurity elements Co, Cr, Fe, Ni, Np, U were found to move in the same direction as the molten zone as predicted by binary phase diagrams. The elements Al, Am, and Ga moved in the opposite direction of the molten zone as predicted by binary phase diagrams. As the impurity alloy was zone refined, {delta}-phase plutonium metal crystals were produced. The first few zone refining passes were more effective than each later pass because an oxide layer formed on the rod surface. There was no clear evidence of better impurity movement at the slower zone refining speed. Also, constant or variable coil power appeared to have no effect on impurity movement during a single run (10 passes). This experiment was the first step to developing a zone refining process for plutonium metal.

  20. Nature of nano-sized plutonium particles in soils at the Hanford site

    Energy Technology Data Exchange (ETDEWEB)

    Buck, Edgar C. [Pacific Northwest National Laboratory, Richland, WA (United States). Energy and Environment Directorate,; Moore, Dean A.; Felmy, Andrew R. [Pacific Northwest National Laboratory, Richland, WA (United States). Fundamental Science Directorate; Czerwinski, Kenneth R. [Nevada Univ., Las Vegas, NV (United States). Harry-Reid Center for Environmental Studies; Conradson, Steven D.; Batuk, Olga N. [Los Alamos National Laboratory, Los Alamos, NM (United States)

    2014-07-01

    The occurrence of plutonium dioxide (PuO{sub 2}) either from direct deposition or from the precipitation of plutonium-bearing solutions in contaminated soils and sediments is well described, particularly for the Hanford site in Washington State. However, past research has suggested that plutonium at the Hanford site may exist in chemical forms in addition to PuO{sub 2}. Although the majority of the plutonium is present as oxide, we present evidence for the formation of nano-sized mixed plutonium- iron phosphate hydroxide structurally related to the rhabdophane group minerals in 216-Z9 crib sediments from Hanford using both transmission electron microscopy (TEM) and X-ray absorption spectroscopy (XAS). The iron-plutonium phosphate formation may depend on the local microenvironment in the sediments, availability of phosphate, and hence the distribution of these minerals may control long-term migration of plutonium in the soil.

  1. /sup 238/Pu fuel form activities, October 1, 1985-March 31, 1986

    Energy Technology Data Exchange (ETDEWEB)

    Ortaldo, J. F.

    1986-07-01

    This report summarizes production of /sup 238/PuO/sub 2/ fuel forms for use in radioisotopic thermoelectric generators (RTG's) in the Plutonium Fuel Form (Puff) Facility at the Savannah River Plant.

  2. Study of Pretreatment Method for Measurement of Small Quantity of U, Np, Pu in 1AW

    Institute of Scientific and Technical Information of China (English)

    DENG; Wei-qin; TAN; Shu-ping; WU; Ji-zong; TAO; Miao-miao

    2012-01-01

    <正>The analysis of U, Np, Pu in 1AW plays an important role on monitoring of plutonium and uranium recovery and neptunium distribution in co-decontamination cycle. Due to the high radioactivity and the

  3. Plutonium-DTPA Model Application with USTUR Case 0269.

    Science.gov (United States)

    Konzen, Kevin; Brey, Richard; Miller, Scott

    2016-01-01

    A plutonium-DTPA (Pu-DTPA) biokinetic model was introduced that had originated from the study of a plutonium-contaminated wound. This work evaluated the extension of the Pu-DTPA model to United States Transuranium and Uranium Registry (USTUR) Case 0269 involving an acute inhalation of a plutonium nitrate aerosol. Chelation was administered intermittently for the first 7 mo as Ca-EDTA, mostly through intravenous injection, with Ca-DTPA treatments administered approximately 2.5 y post intake. Urine and fecal bioassays were collected following intake for several years. Tissues were collected and analyzed for plutonium content approximately 38 y post intake. This work employed the Pu-DTPA model for predicting the urine and fecal bioassay and final tissue quantity at autopsy. The Pu-DTPA model was integrated with two separate plutonium systemic models (i.e., ICRP Publication 67 and its proposed modification). This work illustrated that the Pu-DTPA model was useful for predicting urine and fecal bioassay, including final tissue quantity, 38 y post intake.

  4. Redox reactions of Pu(IV) and Pu(III) in the presence of acetohydroxamic acid in HNO(3) solutions.

    Science.gov (United States)

    Tkac, Peter; Precek, Martin; Paulenova, Alena

    2009-12-21

    The reduction of Pu(IV) in the presence of acetohydroxamic acid (HAHA) was monitored by vis-NIR spectroscopy. All experiments were performed under low HAHA/Pu(IV) ratios, where only the Pu(IV)-monoacetohydroxamate complex and Pu uncomplexed with HAHA were present in relevant concentrations. Time dependent concentrations of all absorbing species were resolved using molar extinction coefficients for Pu(IV), Pu(III), and the Pu(AHA)(3+) complex by deconvolution of spectra. From fitting of the experimental data by rate equations integrated by a numeric method three reactions were proposed to describe a mechanism responsible for the reduction and oxidation of plutonium in the presence of HAHA and HNO(3). Decomposition of Pu(AHA)(3+) follows a second order reaction mechanism with respect to its own concentration and leads to the formation of Pu(III). At low HAHA concentrations, a two-electron reduction of uncomplexed Pu(IV) with HAHA also occurs. Formed Pu(III) is unstable and slowly reoxidizes back to Pu(IV), which, at the point when all HAHA is decomposed, can be catalyzed by the presence of nitrous acid.

  5. Plutonium isotopes in the terrestrial environment at the Savannah River Site, USA: a long-term study.

    Science.gov (United States)

    Armstrong, Christopher R; Nuessle, Patterson R; Brant, Heather A; Hall, Gregory; Halverson, Justin E; Cadieux, James R

    2015-02-01

    This work presents the findings of a long-term plutonium (Pu) study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at the Savannah River National Laboratory (SRNL) in the A-Area. Plutonium content and isotopic abundances were measured over this time period by α particle and thermal ionization mass spectrometry (3STIMS). We detail the complete process of the sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the (238)Pu/(239+240)Pu activity ratios attributed to SRS are substantially different than fallout due to past (238)Pu production on the site. The (240)Pu/(239)Pu atom ratios are reasonably consistent from year to year and are lower than fallout indicating an admixture of weapons-grade material, while the (242)Pu/(239)Pu atom ratios are higher than fallout values, again due to actinide production activities. Overall, the plutonium signatures obtained in this study reflect a distinctive mixture of weapons-grade, heat source, and higher burn-up plutonium with fallout material. This study provides a unique opportunity for developing and demonstrating a blue print for long-term low-level monitoring of trace plutonium in the environment.

  6. PLUTONIUM SOLUBILITY IN HIGH-LEVEL WASTE ALKALI BOROSILICATE GLASS

    Energy Technology Data Exchange (ETDEWEB)

    Marra, J.; Crawford, C.; Fox, K.; Bibler, N.

    2011-01-04

    The solubility of plutonium in a Sludge Batch 6 (SB6) reference glass and the effect of incorporation of Pu in the glass on specific glass properties were evaluated. A Pu loading of 1 wt % in glass was studied. Prior to actual plutonium glass testing, surrogate testing (using Hf as a surrogate for Pu) was conducted to evaluate the homogeneity of significant quantities of Hf (Pu) in the glass, determine the most appropriate methods to evaluate homogeneity for Pu glass testing, and to evaluate the impact of Hf loading in the glass on select glass properties. Surrogate testing was conducted using Hf to represent between 0 and 1 wt % Pu in glass on an equivalent molar basis. A Pu loading of 1 wt % in glass translated to {approx}18 kg Pu per Defense Waste Processing Facility (DWPF) canister, or about 10X the current allowed limit per the Waste Acceptance Product Specifications (2500 g/m{sup 3} of glass or about 1700 g/canister) and about 30X the current allowable concentration based on the fissile material concentration limit referenced in the Yucca Mountain Project License Application (897 g/m{sup 3}3 of glass or about 600 g Pu/canister). Based on historical process throughput data, this level was considered to represent a reasonable upper bound for Pu loading based on the ability to provide Pu containing feed to the DWPF. The task elements included evaluating the distribution of Pu in the glass (e.g. homogeneity), evaluating crystallization within the glass, evaluating select glass properties (with surrogates), and evaluating durability using the Product Consistency Test -- Method A (PCT-A). The behavior of Pu in the melter was evaluated using paper studies and corresponding analyses of DWPF melter pour samples.The results of the testing indicated that at 1 wt % Pu in the glass, the Pu was homogeneously distributed and did not result in any formation of plutonium-containing crystalline phases as long as the glass was prepared under 'well-mixed' conditions

  7. Determination of plutonium content in high burnup pressurized water reactor fuel samples and its use for isotope correlations for isotopic composition of plutonium.

    Science.gov (United States)

    Joe, Kihsoo; Jeon, Young-Shin; Han, Sun-Ho; Lee, Chang-Heon; Ha, Yeong-Keong; Song, Kyuseok

    2012-06-01

    The content of plutonium isotopes in high burnup pressurized water reactor fuel samples was examined using both alpha spectrometry and mass spectrometry after anion exchange separation. The measured values were compared with results calculated by the ORIGEN-2 code. On average, the ratios (m/c) of the measured values (m) over the calculated values (c) were 1.22±0.16 for (238)Pu, 1.02±0.14 for (239)Pu, 1.08±0.06 for (240)Pu, 1.06±0.16 for (241)Pu, and 1.13±0.08 for (242)Pu. Using the Pu data obtained in this work, correlations were derived between the alpha activity ratios of (238)Pu/((239)Pu+(240)Pu), the alpha specific activities of Pu, and the atom % abundances of the Pu isotopes. Using these correlations, the atom % abundances of the plutonium isotopes in the target samples were calculated. These calculated results agreed within a range from 2 to 8% of the experimentally derived values according to the isotopes of plutonium.

  8. Plutonium sorption and desorption behavior on bentonite.

    Science.gov (United States)

    Begg, James D; Zavarin, Mavrik; Tumey, Scott J; Kersting, Annie B

    2015-03-01

    Understanding plutonium (Pu) sorption to, and desorption from, mineral phases is key to understanding its subsurface transport. In this work we study Pu(IV) sorption to industrial grade FEBEX bentonite over the concentration range 10(-7)-10(-16) M to determine if sorption at typical environmental concentrations (≤10(-12) M) is the same as sorption at Pu concentrations used in most laboratory experiments (10(-7)-10(-11) M). Pu(IV) sorption was broadly linear over the 10(-7)-10(-16) M concentration range during the 120 d experimental period; however, it took up to 100 d to reach sorption equilibrium. At concentrations ≥10(-8) M, sorption was likely affected by additional Pu(IV) precipitation/polymerization reactions. The extent of sorption was similar to that previously reported for Pu(IV) sorption to SWy-1 Na-montmorillonite over a narrower range of Pu concentrations (10(-11)-10(-7) M). Sorption experiments with FEBEX bentonite and Pu(V) were also performed across a concentration range of 10(-11)-10(-7) M and over a 10 month period which allowed us to estimate the slow apparent rates of Pu(V) reduction on a smectite-rich clay. Finally, a flow cell experiment with Pu(IV) loaded on FEBEX bentonite demonstrated continued desorption of Pu over a 12 day flow period. Comparison with a desorption experiment performed with SWy-1 montmorillonite showed a strong similarity and suggested the importance of montorillonite phases in controlling Pu sorption/desorption reactions on FEBEX bentonite.

  9. Surface-mediated formation of Pu(IV) nanoparticles at the muscovite-electrolyte interface.

    Science.gov (United States)

    Schmidt, Moritz; Lee, Sang Soo; Wilson, Richard E; Knope, Karah E; Bellucci, Francesco; Eng, Peter J; Stubbs, Joanne E; Soderholm, L; Fenter, P

    2013-12-17

    The formation of Pu(IV)-oxo-nanoparticles from Pu(III) solutions by a surface-enhanced redox/polymerization reaction at the muscovite (001) basal plane is reported, with a continuous increase in plutonium coverage observed in situ over several hours. The sorbed Pu extends >70 Å from the surface with a maximum concentration at 10.5 Å and a total coverage of >9 Pu atoms per unit cell area of muscovite (0.77 μg Pu/cm(2)) (determined independently by in situ resonant anomalous X-ray reflectivity and by ex-situ alpha-spectrometry). The presence of discrete nanoparticles is confirmed by high resolution atomic force microscopy. We propose that the formation of these Pu(IV) nanoparticles from an otherwise stable Pu(III) solution can be explained by the combination of a highly concentrated interfacial Pu-ion species, the Pu(III)-Pu(IV) redox equilibrium, and the strong proclivity of tetravalent Pu to hydrolyze and form polymeric species. These results are the first direct observation of such behavior of plutonium on a naturally occurring mineral, providing insights into understanding the environmental transport of plutonium and other contaminants capable of similar redox/polymerization reactions.

  10. Perturbation in the {sup 240}Pu/{sup 239}Pu global fallout ratio in local sediment following the nuclear accidents at Thule (Greenland) and Palomares (Spain)

    Energy Technology Data Exchange (ETDEWEB)

    Mitchell, P.I.; Vintro, L.L. [University Coll., Dublin (Ireland). Dept. of Physics; Dahlgaard, H. [Risoe National Lab., Roskilde (Denmark); Gasco, C.; Sanchez-Cabeza, J.A. [Barcelona Univ. (Spain). Dept. de Fisica Teorica

    1995-12-31

    It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical {sup 240}Pu/{sup 239}Pu atom ratio of {approx}0.18. Measurements of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing, has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the {sup 240}Pu/{sup 239}Pu ratio has been examined in samples of sediment collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The {sup 240}Pu/{sup 239}Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution. The analytical results showed that at Thule the mean {sup 240}Pu/{sup 239}Pu atom ratio was 0.033{+-}0.004, while at Palomares the equivalent ratio appeared to be significantly higher at 0.056{+-}0.003. Both ratios are consistent with those reported for soils samples at the Nevada site and Nagasaki, and are clearly indicative of weapons-grade plutonium. 27 refs., 1 fig., 2 tabs.

  11. Methodological Study on AMS Measurement of Ultra-trace Pu Isotope Ratios at CIAE

    Institute of Scientific and Technical Information of China (English)

    DONG; Ke-jun; ZHAO; Qing-zhang; WANG; Chen; HE; Ming; JIANG; Shan; ZHANG; Hui; PANG; Yi-jun; SHEN; Hong-tao; WANG; Xiao-ming; XU; Yong-ning; WU; Shao-yong; YANG; Xu-ran; WANG; Xiang-gao

    2015-01-01

    The determination of ultra-trace plutonium is very important in different fields.A new measurement method of plutonium isotopic ratios with accelerator mass spectrometry(AMS)was developed at China Institute of Atomic Energy(CIAE).Two laboratory reference standards of 239Pu/240 Pu(ST1)and 239Pu/242 Pu(ST2)are17.241and 10.059,a flow blank,a commercial blank and three real samples were respectively

  12. Plutonium in monazite and brabantite: Diffuse reflectance spectroscopy study

    Energy Technology Data Exchange (ETDEWEB)

    Zhang Yingjie [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, PMB 1, Menai, NSW 2234 (Australia)], E-mail: yzx@ansto.gov.au; Vance, Eric R. [Institute of Materials Engineering, Australian Nuclear Science and Technology Organisation, PMB 1, Menai, NSW 2234 (Australia)

    2008-04-30

    The valence states of plutonium (Pu) in monazite and brabantite have been studied by using diffuse reflectance spectroscopy. In the absence of charge compensators, Pu exists mainly as trivalent ions in air-fired monazites and only trivalent ions in argon-fired monazites. However, with added Ca{sup 2+}/Pb{sup 2+} as charge compensators Pu can exist as tetravalent ions. Published data on absorption spectra of both trivalent and tetravalent Pu ions in the monazite structure have been extended to the mid near infrared region (4000 cm{sup -1})

  13. Design of the Laboratory-Scale Plutonium Oxide Processing Unit in the Radiochemical Processing Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Lumetta, Gregg J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Meier, David E. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Tingey, Joel M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Casella, Amanda J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Delegard, Calvin H. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Edwards, Matthew K. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Orton, Robert D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Rapko, Brian M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Smart, John E. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-05-01

    This report describes a design for a laboratory-scale capability to produce plutonium oxide (PuO2) for use in identifying and validating nuclear forensics signatures associated with plutonium production, as well as for use as exercise and reference materials. This capability will be located in the Radiochemical Processing Laboratory at the Pacific Northwest National Laboratory. The key unit operations are described, including PuO2 dissolution, purification of the Pu by ion exchange, precipitation, and re-conversion to PuO2 by calcination.

  14. Electrochemical studies on plutonium in molten salts

    Energy Technology Data Exchange (ETDEWEB)

    Bourges, G. [CEA-Centre d' etudes de Valduc, 21 120 Is sur Tille (France)], E-mail: gilles.bourges@cea.fr; Lambertin, D.; Rochefort, S. [CEA-Centre d' etudes de Valduc, 21 120 Is sur Tille (France); Delpech, S.; Picard, G. [Laboratoire d' Electrochimie et de Chimie Analytique (UMR7575, CNRS), ENSCP, 11 rue Pierre et Marie Curie, 75231 Paris (France)

    2007-10-11

    Electrochemical studies on plutonium have been supporting the development of pyrochemical processes involving plutonium at CEA. The electrochemical properties of plutonium have been studied in molten salts - ternary eutectic mixture NaCl-KCl-BaCl{sub 2}, equimolar mixture NaCl-KCl and pure CaCl{sub 2} - and in liquid gallium at 1073 K. The formal, or apparent, standard potential of Pu(III)/Pu redox couple in eutectic mixture of NaCl-KCl-BaCl{sub 2} at 1073 K determined by potentiometry is equal to -2.56 V (versus Cl{sub 2}, 1 atm/Cl{sup -} reference electrode). In NaCl-KCl eutectic mixture and in pure CaCl{sub 2} the formal standard potentials deduced from cyclic voltammetry are respectively -2.54 V and -2.51 V. These potentials led to the calculation of the activity coefficients of Pu(III) in the molten salts. Chronoamperometry on plutonium in liquid gallium using molten chlorides - CaCl{sub 2} and equimolar NaCl/KCl - led to the determination of the activity coefficient of Pu in liquid Ga, log {gamma} = -7.3. This new data is a key parameter to assess the thermodynamic feasibility of a process using gallium as solvent metal. By comparing gallium with other solvent metals - cadmium, bismuth, aluminum - gallium appears to be, with aluminum, more favorable for the selectivity of the separation at 1073 K of plutonium from cerium. In fact, compared with a solid tungsten electrode, none of these solvent liquid metals is a real asset for the selectivity of the separation. The role of a solvent liquid metal is mainly to trap the elements.

  15. The concentrations of 241Pu in the southern Baltic Sea

    Directory of Open Access Journals (Sweden)

    Strumińska-Parulska D. I.

    2013-04-01

    Full Text Available The aim of the work was 241Pu activities determination in different components (water, plankton and fish of the southern Baltic Sea ecosystem. The determination of 241Pu in the samples was done indirectly by activity measuring the increment in 241Am from the decay of β-emitting 241Pu in samples collected 10-15 years after the Chernobyl accident. Enhanced levels of 241Pu were observed in all analyzed Baltic samples. The plutonium is also non-uniformly distributed between the organs and tissues of the analyzed fish; especially pelagic herring and cod as well as benthic flounder. The annual individual effective doses calculated on the basis of 241Pu concentrations in fish indicated that the impact of the consumption of 241Pu with Baltic fish on the annual effective dose for a statistical inhabitant of Poland was very small.

  16. Application of laser-induced photoacoustic spectroscopy for determination of plutonium concentration in nuclear waste solutions.

    Science.gov (United States)

    Surugaya, Naoki; Sato, Soichi; Jitsukata, Syu; Watahiki, Masaru

    2008-04-01

    Laser-induced photoacoustic spectroscopy was used in a quantitative analysis of Pu in HNO3 medium. Plutonium was quantitatively oxidized to Pu(VI) using Ce(IV). The photoacoustic measurement of Pu(VI) with maximum absorption at 830.5 nm was subsequently performed to determine the concentration. The photoacoustic signal was linearly proportional to the Pu(VI) ion concentration. The detection limit of Pu(VI) was estimated to be 0.5 microg mL(-1) (3sigma) in 3 M HNO3. By the proposed method, Pu concentration was successfully determined in a nuclear waste solution for use in nuclear materials management.

  17. ``Distribution and behaviour of plutonium in the waters of the channel and of the seine estuary``; ``Distribution et comportement du plutonium dans les eaux de la manche et de l`estuaire de la seine``

    Energy Technology Data Exchange (ETDEWEB)

    Garcia, K.

    1997-12-31

    Excess dissolved plutonium has been measured in the coastal waters of the Channel, from Granville to Boulogne, probably due to sorption-desorption processus. In the Seine estuary, in situ measurements and experimental studies showed that the plutonium desorbs himself from particles in low salinity waters. The desorbed plutonium originates in marine and/or fluvial dissolved Pu. Marine dissolved Pu(V), originating from La Hague plant discharges and from atlantic waters, is reduced and sorbed when the salinity decreases onto estuarial particles: Isotopic Activity Ration {sup 238}Pu/{sup 239}, Pu(IR) of marine dissolved Pu(V) is about 0.7. Fluvial dissolved plutonium originates from atmospheric fallout and from an internal river source: fallout plutonium (IR=0.05) is unreactive with salinity while 45% of river plutonium (IR>1.7) flocculates at 0.5 g l{sup -1}. Desorbed plutonium may have various origins, depending on the Seine liquid discharges and on the tidal coefficient. When the marine waters do not migrate upstream, the low salinity waters encounters particles marked essentially with marine plutonium and the IR of desorbed Pu is about 0.7. The activities of desorbed plutonium are too low to have any influence on the distribution of plutonium in the coastal waters on the Seine Bay. When the marine waters migrate upstream, the low salinity waters meet particles marked essentially with river plutonium (IR>1.7) and desorbed plutonium has a very high IR. These estuarine conditions are encountered five to seven month a year and implicate an increase of the IR of 0.1 of the plutonium present in the coastal waters of the Seine bay (1.2.-1.3.). (author).

  18. Economical Production of Pu-238

    Energy Technology Data Exchange (ETDEWEB)

    Steven D. Howe; Douglas Crawford; Jorge Navarro; Terry Ring

    2013-02-01

    All space exploration missions traveling beyond Jupiter must use radioisotopic power sources for electrical power. The best isotope to power these sources is plutonium-238. The US supply of Pu-238 is almost exhausted and will be gone within the next decade. The Department of Energy has initiated a production program with a $10M allocation from NASA but the cost is estimated at over $100 M to get to production levels. The Center for Space Nuclear Research has conceived of a potentially better process to produce Pu-238 earlier and for significantly less cost. The new process will also produce dramatically less waste. Potentially, the front end costs could be provided by private industry such that the government only had to pay for the product produced. Under a NASA Phase I NIAC grant, the CSNR has evaluated the feasibility of using a low power, commercially available nuclear reactor to produce at least 1.5 kg of Pu-238 per year. The impact on the neutronics of the reactor have been assessed, the amount of Neptunium target material estimated, and the production rates calculated. In addition, the size of the post-irradiation processing facility has been established. In addition, a new method for fabricating the Pu-238 product into the form used for power sources has been identified to reduce the cost of the final product. In short, the concept appears to be viable, can produce the amount of Pu-238 needed to support the NASA missions, can be available within a few years, and will cost significantly less than the current DOE program.

  19. Imitators of plutonium and americium in a mixed uranium- plutonium nitride fuel

    Science.gov (United States)

    Nikitin, S. N.; Shornikov, D. P.; Tarasov, B. A.; Baranov, V. G.; Burlakova, M. A.

    2016-04-01

    Uranium nitride and mix uranium nitride (U-Pu)N is most popular nuclear fuel for Russian Fast Breeder Reactor. The works in hot cells associated with the radiation exposure of personnel and methodological difficulties. To know the main physical-chemical properties of uranium-plutonium nitride it necessary research to hot cells. In this paper, based on an assessment of physicochemical and thermodynamic properties of selected simulators Pu and Am. Analogues of Pu is are Ce and Y, and analogues Am - Dy. The technique of obtaining a model nitride fuel based on lanthanides nitrides and UN. Hydrogenation-dehydrogenation- nitration method of derived powders nitrides uranium, cerium, yttrium and dysprosium, held their mixing, pressing and sintering, the samples obtained model nitride fuel with plutonium and americium imitation. According to the results of structural studies have shown that all the samples are solid solution nitrides rare earth (REE) elements in UN.

  20. Plutonium Speciation in Support of Oxidative-Leaching Demonstration Test

    Energy Technology Data Exchange (ETDEWEB)

    Sinkov, Sergey I.

    2007-10-31

    Bechtel National, Inc. (BNI) is evaluating the plutonium speciation in caustic solutions that reasonably represent the process streams from the oxidative-leaching demonstration test. Battelle—Pacific Northwest Division (PNWD) was contracted to develop a spectrophotometric method to measure plutonium speciation at submicromolar (< 10-6 M) concentrations in alkaline solutions in the presence of chromate and carbonate. Data obtained from the testing will be used to identify the oxidation state of Pu(IV), Pu(V), and Pu(VI) species, which potentially could exist in caustic leachates. Work was initially conducted under contract number 24590-101-TSA-W000-00004 satisfying the needs defined in Appendix C of the Research and Technology Plan TSS A-219 to evaluate the speciation of chromium, plutonium, and manganese before and after oxidative leaching. In February 2007, the contract mechanism was switched to Pacific Northwest National Laboratory (PNNL) Operating Contract MOA: 24590-QL-HC9-WA49-00001.

  1. MICROBIAL TRANSFORMATIONS OF PLUTONIUM AND IMPLICATIONS FOR ITS MOBILITY.

    Energy Technology Data Exchange (ETDEWEB)

    FRANCIS, A.J.

    2000-09-30

    The current state of knowledge of the effect of plutonium on microorganisms and microbial activity is reviewed, and also the microbial processes affecting its mobilization and immobilization. The dissolution of plutonium is predominantly due to their production of extracellular metabolic products, organic acids, such as citric acid, and sequestering agents, such as siderophores. Plutonium may be immobilized by the indirect actions of microorganisms resulting in changes in Eh and its reduction from a higher to lower oxidation state, with the precipitation of Pu, its bioaccumulation by biomass, and bioprecipitation reactions. In addition, the abundance of microorganisms in Pu-contaminated soils, wastes, natural analog sites, and backfill materials that will be used for isolating the waste and role of microbes as biocolloids in the transport of Pu is discussed.

  2. Slowdown Trade Surplus Growth

    Institute of Scientific and Technical Information of China (English)

    Leo Zhao

    2008-01-01

    @@ According to Ma Kai's economic planning report submitted to the NPC session on March 5th.(Ma Kai is the Minister in charge of the National Development and Reform Commission),the government has listed the slowdown in trade surplus growth and the steady expansion of,external investment as major tasks for 2008.

  3. 'Nonprofits' need surplus too.

    Science.gov (United States)

    Young, D W

    1982-01-01

    By definition profit refers to the difference between revenue and expenses. In for-profit organizations profit or surplus gives a return to the owners of the company and serves as a source of financing for capital acquisitions and working capital. Nonprofit organizations, which are not allowed a surplus, don't suffer on the first count because they have no owners. But they do suffer on the second count because, if expected to grow, they need to finance asset replacement and growth. In these days when funds for long-term debt are becoming scarcer, this author asserts, the need for regulators to allow 'nonprofits' to keep a surplus is increasing. In this article, he argues for a surplus and then discusses how managers and regulators can determine how much a nonprofit organization should be allowed. He presents a combination of a modified version of the return-on-asset pricing model used in for-profit organizations and a model for assessing working capital needs associated with growth.

  4. Racism and Surplus Repression.

    Science.gov (United States)

    Johnson, Howard

    1983-01-01

    Explores the relationship between Herbert Marcuse's theory of "surplus repression" and Freud's theory of the "unconscious" with respect to latent, hidden, covert, or subliminal aspects of racism in the United States. Argues that unconscious racism, manifested in evasion/avoidance, acting out/projection, and attempted justification, perpetuates…

  5. Plutonium immobilization plant using glass in new facilities at the Savannah River Site

    Energy Technology Data Exchange (ETDEWEB)

    DiSabatino, A.

    1998-06-01

    The Plutonium Immobilization Plant (PIP) accepts plutonium (Pu) from pit conversion and from non-pit sources and, through a glass immobilization process, converts the plutonium into an immobilized form that can be disposed of in a high level waste (HLW) repository. This immobilization process is shown conceptually in Figure 1-1. The objective is to make an immobilized form, suitable for geologic disposal, in which the plutonium is as inherently unattractive and inaccessible as the plutonium in spent fuel from commercial reactors.

  6. The interaction of Desulfovibrio aespoeensis DSM 10631{sup T} with plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Moll, H.; Merroun, M.L.; Hennig, C.; Rossberg, A.; Selenska-Pobell, S.; Bernhard, G. [Inst. fuer Radiochemie, Forschungszentrum Rossendorf e.V., Dresden (Germany)

    2006-07-01

    Microbes are widely distributed in nature and they can strongly influence the migration of actinides in the environment. This investigation describes the interaction of plutonium in mixed oxidation states (Pu(VI) and Pu(IV)-polymers) with cells of the sulfate-reducing bacterial (SRB) strain Desulfovibrio aespoeensis DSM 10631{sup T}, which frequently occurs in the deep granitic rock aquifers at the AespoeHard Rock Laboratory (AespoeHRL), Sweden. In this study, accumulation experiments were performed in order to obtain information about the amount of Pu bound by the bacteria in dependence on the contact time and the initial plutonium concentration. We used solvent extractions, UV-Vis absorption spectroscopy and X-ray absorption near edge structure (XANES) spectroscopy to determine the speciation of Pu oxidation states. Extended X-ray absorption fine structure (EXAFS) spectroscopy was used to study the coordination of the Pu bound by the bacteria. In the first step, the Pu(VI) and Pu(IV)-polymers are bound to the biomass. Solvent extractions showed that 97% of the initially present Pu(VI) is reduced to Pu(V) due to the activity of the cells within the first 24 h of contact time. Most of the formed Pu(V) dissolves from the cell envelope back to the aqueous solution due to the weak complexing properties of this plutonium oxidation state. Indications were found for a penetration of Pu species inside the bacterial cells. (orig.)

  7. Occurrence of plutonium in the terrestrial environment at Thule, Greenland

    DEFF Research Database (Denmark)

    Roos, Per; Jernström, Jussi; Nielsen, Sven Poul

    2011-01-01

    to several hundred kBq per m2 of Pu. Although concentrations in surface soil can be very high the concentration in analysed air filter samples and passive aerosol collectors are very low. Exposure to plutonium due to inhalation of airborne plutonium particles in the area is of little importance according...... to this study. To further assess the risk of inhaling resuspended material particles isolated from the different hot areas have been subject to investigation on stability and leaching behaviour....

  8. Preparation of Plutonium Counting Source Using Solid Phase Extraction Disk

    Institute of Scientific and Technical Information of China (English)

    SUN; Hong-qing; YANG; Su-liang; DING; You-qian; YANG; Jin-ling; MAO; Guo-shu

    2013-01-01

    For the determination of trace amount of plutonium,Pu(Ⅳ)may be extracted from dilute nitric acid by TTA-xylene,and stripped by concentrated nitric acid.But the small volume of strip solution used in traditional counting source preparation by direct evaporation could lead to a rather high detection limit.Plutonium in strip solution may all be absorbed on the surface of an anion exchange resin disk.And

  9. Synthesis of Pu-Doped Ceramic

    Energy Technology Data Exchange (ETDEWEB)

    Anderson, E. B

    1998-09-02

    Plutonium-doped zircon containing about 10 wt% Pu was synthesized in this cooperative project between Russia and the United States conducted at the V. G. Khlopin Radium Institute. The sol-gel method was used for starting precursor preparation to provide complete mixing of initial components and to avoid dust formation inside the glove-box. The sol-gel process also gives interim Pu stabilization in the form of amorphous zirconium hydrosilicate (AZHS), which is a result of gel solidification. AZHS is a solid and relatively durable material that can be easy converted into crystalline zircon by pressureless sintering, thus avoiding significant radioactive contamination of laboratory equipment. A methanol-aqueous solution of tetraethoxysilane Si(OC2H5)4, Pu-nitrate, and zirconil oxynitrate was prepared in final stoichiometry of zircon (Zr,Pu)SiO4 80 wt% + zirconia (Zr,Pu)O2 20 wt%. Gelation occurred after 90 hours at room temperature. AZHS with excess of zirconia 20 wt% was obtained as an interim calcine product and then it was converted into zircon/zirconia ceramic by sintering at 1490 to 1500°C in air for different time periods. The samples obtained were studied by SRD and ESEM methods. It was found that both zircon yield and zircon cell parameters that are correlated with Pu incorporation depend on sintering time.

  10. Geochemical association of plutonium in marine sediments from Palomares (Spain)

    Energy Technology Data Exchange (ETDEWEB)

    Anton, M.P. [Dept. de Geoquimica e Impacto Ambiental, CIEMAT, Madrid (Spain); Gasco, C. [Dept. de Geoquimica e Impacto Ambiental, CIEMAT, Madrid (Spain); Sanchez-Cabeza, J.A. [Dept. de Fisica, Univ. Autonoma de Barcelona (Spain); Pujol, L. [Dept. de Fisica, Univ. Autonoma de Barcelona (Spain)

    1994-12-31

    The geochemical association of plutonium in sediments from the marine ecosystem of Palomares has been studied. A sequential leaching technique using selective extractants has been employed to determine the percentages of Pu in the following forms: (a) readily available, (b) exchangeable and adsorbed to specific sites, (c) associated with organic matter, (d) sesquioxides, (e) residual. Plutonium was found to be associated mainly with phases (c), (d) and (e), and therefore, appears to be relatively immobile and not readily available to bottom feeding biota. The effect of different source terms on Pu distribution is also discussed. (orig.)

  11. Long term plutonium solubility and speciation studies in a synthetic brine

    Energy Technology Data Exchange (ETDEWEB)

    Nitsche, Heino; Roberts, K.; Xi, Ruihua [Lawrence Berkeley Lab., CA (United States)] [and others

    1993-12-31

    The rate at which elements can be transported in groundwater systems is governed in part by the solubility of the element in the groundwater. This report documents plutonium solubility experiments in a brine simulant relevant to the Waste Isolation Pilot Plant. Approximately 1 to 2.5 mL of five stock solutions containing single oxidation states of plutonium (Pu(IV)-polymer, Pu{sup 3+}, Pu{sup 4+}, PuO{sub 2}{sup +}, and PuO{sub 2}{sup 2+}) were added to {approximately}75 mL of synthetic H-17 Brine in five reaction vessels. Initial plutonium concentrations ranged from 1.3 {times} l0{sup {minus}4} to 5.l {times} l0{sup {minus}4} M (moles per liter) total plutonium. Because these initial concentrations were far above the plutonium solubility limit in H-17 Brine, plutonium-containing solids precipitated. Aqueous plutonium concentrations were measured over time until steady-state was reached, requiring over 300 days in H-17 Brine.

  12. Neutron powder diffraction study of 239PuD x

    Science.gov (United States)

    Bartscher, W.; Boeuf, A.; Caciuffo, R.; Fournier, J. M.; Haschke, J. M.; Manes, L.; Rebizant, J.; Rustichelli, F.; Ward, J. W.

    1985-05-01

    A neutron powder diffraction study has been carried out on several deuterids of Plutonium (PuD 2.25,PuD 2.33, PuD 2.65) to determine the positions of deuterium atoms in the host metal f.c.c. lattice. It has been found that vacancies occur in the tetrahedral sites. Moreover, with increasing deuterium concentration, octahedral interstitial deuterium atoms are displaced from their ideal positions. These results can be explained by the formation of clusters. Finally, at low temperature, these compounds become ferromagnetically ordered. An ordered magnetic moment μ 0≈0.8 μ B has been measured on all compounds.

  13. The structure of plutonium(IV) oxide as hydrolysed clusters in aqueous suspensions.

    Science.gov (United States)

    Ekberg, Christian; Larsson, Kristian; Skarnemark, Gunnar; Ödegaard-Jensen, Arvid; Persson, Ingmar

    2013-02-14

    The behavior of plutonium still puzzles scientists 70 years after its discovery. There are several factors making the chemistry of plutonium interesting including its ability to keep several oxidation states. Another unique property is that the oxidation states +III, +IV, +V and +VI may exist simultaneously in solution. Another property plutonium shares with some other tetravalent metal ions is the ability to form stable polynuclear complexes or colloids. The structures of freshly prepared and five-year old plutonium(IV) colloids are compared with crystalline plutonium(IV) oxide using Pu L(3)-edge EXAFS. It was shown that as the plutonium colloids age they do in fact shrink in size, contrary to previous expectations. The aged colloidal particles are indeed very small with only 3-4 plutonium atoms, and with a structure very similar to solid plutonium(IV) oxide, but with somewhat shorter mean Pu-O bond and Pu···Pu distances indicating a partial oxidation. The very small size of the colloidal particles is further supported by the fact that they do not sediment on heavy ultra-centrifugation.

  14. Plutonium and americium contamination in Rocky Flats soil, 1973

    Energy Technology Data Exchange (ETDEWEB)

    Krey, P.; Hardy, E.; Volchok, H.; Toonkel, L.; Knuth, R.; Coppes, M.; Tamura, T.

    1976-03-01

    The plutonium mass isotopic analysis and the Am-241 analysis of soil samples from Rocky Flats identify the contamination as Pu which was processed in 1958. The Am-241 activity in the soil will reach its maximum in 2033 and represent 18 percent of the Pu-239-240 activity. Nuclide ratios indicate that current operations at Rocky Flats contribute little to the airborne Pu concentrations which are due to resuspension of the contaminated soil. Root uptake of Pu or Am by vegetation is slight or shows no discrimination among the isotopes and nuclides studied. The relationship between Pu deposition contour and the area enclosed by that contour has been verified for contour values extending over 7 orders of magnitude. This gives confidence to our calculations of the quantities of Pu released on and off the Rocky Flats plant site. (auth)

  15. Anticipated Radiological Dose to Worker for Plutonium Stabilization and Handling at PFP - Project W-460

    CERN Document Server

    Weiss, E V

    2000-01-01

    This report provides estimates of the expected whole body and extremity radiological dose, expressed as dose equivalent (DE), to workers conducting planned plutonium (Pu) stabilization processes at the Hanford Site Plutonium Finishing Plant (PFP). The report is based on a time and motion dose study commissioned for Project W-460, Plutonium Stabilization and Handling, to provide personnel exposure estimates for construction work in the PFP storage vault area plus operation of stabilization and packaging equipment at PFP.

  16. Density-functional study of plutonium monoxide monohydride

    Science.gov (United States)

    Qiu, Ruizhi; Lu, Haiyan; Ao, Bingyun; Tang, Tao; Chen, Piheng

    2017-03-01

    The structural, electronic, mechanical, optical, thermodynamic properties of plutonium monoxide monohydride (PuOH) are studied by density-functional calculations within the framework of LDA/GGA and LDA/GGA+U. From the total energy calculation, the lowest-energy crystal structure of PuOH is predicted to have space group F 4 bar 3 m (No. 216). Within the LDA+U framework, the calculated lattice parameter of F 4 bar 3 m -PuOH is in good agreement with the experimental value and the corresponding ground state is predicted to be an antiferromagnetic charge-transfer insulator. Furthermore, we investigate the bonding character of PuOH by analyzing the electron structure and find that there are a stronger Pu-O bond and a weaker Pu-H bond. The mechanical properties including the elastic constants, elastic moduli and Debye's temperature, and the optical properties including the reflectivity and absorption coefficient are also calculated. We then compute the phonon spectrum which verified the dynamical stability of F 4 bar 3 m -PuOH. Some thermodynamic quantities such as the specific heat are evaluated. Finally we calculate the formation energy of PuOH, and the reaction energies for the oxidation of PuOH and PuOH-coated Pu, which are in reasonable agreement with the experimental values.

  17. Standard test method for plutonium assay by plutonium (III) diode array spectrophotometry

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2002-01-01

    1.1 This test method describes the determination of total plutonium as plutonium(III) in nitrate and chloride solutions. The technique is applicable to solutions of plutonium dioxide powders and pellets (Test Methods C 697), nuclear grade mixed oxides (Test Methods C 698), plutonium metal (Test Methods C 758), and plutonium nitrate solutions (Test Methods C 759). Solid samples are dissolved using the appropriate dissolution techniques described in Practice C 1168. The use of this technique for other plutonium-bearing materials has been reported (1-5), but final determination of applicability must be made by the user. The applicable concentration range for plutonium sample solutions is 10–200 g Pu/L. 1.2 The values stated in SI units are to be regarded as standard. No other units of measurement are included in this standard. 1.3 This standard does not purport to address all of the safety concerns, if any, associated with its use. It is the responsibility of the user of this standard to establish appropria...

  18. Studies of the ternary systems humic substances - kaolinite - Pu(III) and Pu(IV)

    Energy Technology Data Exchange (ETDEWEB)

    Buda, R.A.; Kratz, J.V.; Trautmann, N. [Inst. fuer Kernchemie, Johannes-Gutenberg-Univ., Mainz (Germany); Banik, N.L. [Inst. fuer Kernchemie, Johannes-Gutenberg-Univ., Mainz (Germany); Inst. fuer Nukleare Entsorgung (INE), Forschungszentrum Karlsruhe (Germany)

    2008-07-01

    The behaviour of plutonium with respect to its migration in the aquifer has been studied under conditions close to nature. Most relevant under these conditions are Pu(III) and Pu(IV) in contact with humic substances (HS) and minerals. As a model for the host rock, kaolinite (KGa-1b) was chosen. The complexation of Pu(III) and Pu(IV) with Aldrich humic acid (AHA) in aqueous solution at ionic strength 0.1 M was investigated by the ultrafiltration method. The sorption of Pu(III) and Am(III) onto kaolinite (K) as a function of pH and metal-ion concentration was studied under aerobic and anaerobic conditions. The pH edge was found at pH {proportional_to} 5.5 independent of the metal-ion concentration and working atmosphere. The influence of HS on the sorption of Pu(III) and Pu(IV) onto kaolinite was investigated in the ternary systems Pu(III)-K-HS and Pu(IV)-K-HS and for comparison, in the system Th(IV)-K-HS. The dependence on pH, contact time, concentration of HS (for Pu(IV)-K-HS) was studied as well as the sequence in which the components were added. Generally, it was found that HS tend to enhance the sorption onto kaolinite below pH 6 and to decrease sorption at higher pH depending in detail on the sequence in which the components were added. An identification of the species sorbed on the surface of the kaolinite by X-ray absorption spectroscopy, as well as chemically, was attempted and preliminary results are discussed. (orig.)

  19. Distribution characteristics of ¹³⁷Cs, Pu isotopes and ²⁴¹Am in soil in Korea.

    Science.gov (United States)

    Lee, S H; Oh, J S; Lee, J M; Lee, K B; Park, T S; Lujaniene, G; Valiulis, D; Sakalys, J

    2013-11-01

    Cesium-137, Plutonium isotopes and (241)Am were studied in soil samples collected from Korea between 2006 and 2008 to provide information on the distribution and origin of Pu isotopes and (241)Am. The vertical profiles of radionuclides showed higher activity concentrations at the surface layer and then gradually decreased with depth. A good correlation between (137)Cs and (239,240)Pu was observed, whereas a poor relationship between (137)Cs and (241)Am was found. The (238)Pu/(239,240)Pu, (241)Am/(239,240)Pu and (239,240)Pu/(137)Cs activity ratios were concordant to those of the global fallout ratios. Furthermore, the atomic ratios of (240)Pu/(239)Pu in the samples provided the information of Pu depositional history and the origin of Pu isotopes in Korea.

  20. Uptake and translocation of plutonium in two plant species using hydroponics.

    Science.gov (United States)

    Lee, J H; Hossner, L R; Attrep, M; Kung, K S

    2002-01-01

    This study presents determinations of the uptake and translocation of Pu in Indian mustard (Brassica juncea) and sunflower (Helianthus annuus) from Pu contaminated solution media. The initial activity levels of Pu were 18.50 and 37.00 Bq ml(-1), for Pu-nitrate [239Pu(NO3)4] and for Pu-citrate [239Pu(C6H5O7)+] in nutrient solution. Plutonium-diethylenetriaminepentaacetic acid (DTPA: [239Pu-C14H23O10N3] solution was prepared by adding 0, 5, 10, and 50 microg of DTPA ml(-1) with 239Pu(NO3)4 in nutrient solution. Concentration ratios (CR, Pu concentration in dry plant material/Pu concentration in nutrient solution) and transport indices (Tl, Pu content in the shoot/Pu content in the whole plant) were calculated to evaluate Pu uptake and translocation. All experiments were conducted in hydroponic solution in an environmental growth chamber. Plutonium concentration in the plant tissue was increased with increased Pu contamination. Plant tissue Pu concentration for Pu-nitrate and Pu-citrate application was not correlated and may be dependent on plant species. For plants receiving Pu-DTPA, the Pu concentration was increased in the shoots but decreased in the roots resulting in a negative correlation between the Pu concentrations in the plant shoots and roots. The Pu concentration in shoots of Indian mustard was increased for application rates up to 10 microg DTPA ml(-1) and up to 5 microg DTPA ml(-1) for sunflower. Similar trends were observed for the CR of plants compared to the Pu concentration in the shoots and roots, whereas the Tl was increased with increasing DTPA concentration. Plutonium in shoots of Indian mustard was up to 10 times higher than that in shoots of sunflower. The Pu concentration in the apparent free space (AFS) of plant root tissue of sunflower was more affected by concentration of DTPA than that of Indian mustard.

  1. Radiation-induced non-equilibrium redox chemistry of plutonium: implications for environmental migration

    Energy Technology Data Exchange (ETDEWEB)

    Haschke, J M; Siekhaus, W J

    2009-02-11

    Static concentrations of plutonium oxidation states in solution and at surfaces in oxide-water systems are identified as non-equilibrium steady states. These kinetically controlled systems are described by redox cycles based on irreversible disproportionation of Pu(IV), Pu(V), and Pu(VI) in OH-bridged intermediate complexes and at OH-covered oxide surfaces. Steady state is fixed by continuous redox cycles driven by radioactivity-promoted electron-transfer and energetically favorable reactions of Pu(III) and Pu(VII) disproportionation products with H2O. A model based on the redox cycles accounts for the high steady-state [Pu] coexisting with Pu(IV) hydrous oxide at pH 0-15 and for predominance of Pu(V) and Pu(VI) in solution. The steady-state [Pu] depends on pH and the surface area of oxide in solution, but not on the initial Pu oxidation state. PuO{sub 2+x} formation is attributed to high Pu(V) concentrations existing at water-exposed oxide surfaces. Results infer that migration of Pu in an aqueous environment is controlled by kinetic factors unique to that site and that the predominant oxidation states in solution are Pu(V) and Pu(VI).

  2. Radiation-induced non-equilibrium redox chemistry of plutonium: implications for environmental migration

    Energy Technology Data Exchange (ETDEWEB)

    Haschke, J M; Siekhaus, W J

    2009-02-11

    Static concentrations of plutonium oxidation states in solution and at surfaces in oxide-water systems are identified as non-equilibrium steady states. These kinetically controlled systems are described by redox cycles based on irreversible disproportionation of Pu(IV), Pu(V), and Pu(VI) in OH-bridged intermediate complexes and at OH-covered oxide surfaces. Steady state is fixed by continuous redox cycles driven by radioactivity-promoted electron-transfer and energetically favorable reactions of Pu(III) and Pu(VII) disproportionation products with H2O. A model based on the redox cycles accounts for the high steady-state [Pu] coexisting with Pu(IV) hydrous oxide at pH 0-15 and for predominance of Pu(V) and Pu(VI) in solution. The steady-state [Pu] depends on pH and the surface area of oxide in solution, but not on the initial Pu oxidation state. PuO{sub 2+x} formation is attributed to high Pu(V) concentrations existing at water-exposed oxide surfaces. Results infer that migration of Pu in an aqueous environment is controlled by kinetic factors unique to that site and that the predominant oxidation states in solution are Pu(V) and Pu(VI).

  3. FORM AND AGING OF PLUTONIUM IN SAVANNAH RIVER SITE WASTE TANK 18

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.

    2012-02-24

    This report provides a summary of the effects of aging on and the expected forms of plutonium in Tank 18 waste residues. The findings are based on available information on the operational history of Tank 18, reported analytical results for samples taken from Tank 18, and the available scientific literature for plutonium under alkaline conditions. These findings should apply in general to residues in other waste tanks. However, the operational history of other waste tanks should be evaluated for specific conditions and unique operations (e.g., acid cleaning with oxalic acid) that could alter the form of plutonium in heel residues. Based on the operational history of other tanks, characterization of samples from the heel residues in those tanks would be appropriate to confirm the form of plutonium. During the operational period and continuing with the residual heel removal periods, Pu(IV) is the dominant oxidation state of the plutonium. Small fractions of Pu(V) and Pu(VI) could be present as the result of the presence of water and the result of reactions with oxygen in air and products from the radiolysis of water. However, the presence of Pu(V) would be transitory as it is not stable at the dilute alkaline conditions that currently exists in Tank 18. Most of the plutonium that enters Savannah River Site (SRS) high-level waste (HLW) tanks is freshly precipitated as amorphous plutonium hydroxide, Pu(OH){sub 4(am)} or hydrous plutonium oxide, PuO{sub 2(am,hyd)} and coprecipitated within a mixture of hydrous metal oxide phases containing metals such as iron, aluminum, manganese and uranium. The coprecipitated plutonium would include Pu{sup 4+} that has been substituted for other metal ions in crystal lattice sites, Pu{sup 4+} occluded within hydrous metal oxide particles and Pu{sup 4+} adsorbed onto the surface of hydrous metal oxide particles. The adsorbed plutonium could include both inner sphere coordination and outer sphere coordination of the plutonium. PuO{sub 2

  4. Synthesis and Structural Characterization of a Molecular Plutonium(IV) Compound Constructed from Dimeric Building Blocks

    Energy Technology Data Exchange (ETDEWEB)

    Runde, Wolfgang; Brodnax, Lia F.; Goff, George S.; Peper, Shane M.; Taw, Felicia L.; Scott, Brian L.

    2007-04-01

    Single crystals of Na8Pu2(O2)2(CO3)6•12H2O, exhibiting mu2, eta2-O2 ligands in unprecedented Pu(IV) dimeric units, were obtained at ambient temperature from aqueous Plutonium(IV) peroxide carbonate solution.

  5. SEPARATION OF PLUTONIUM

    Science.gov (United States)

    Maddock, A.G.; Smith, F.

    1959-08-25

    A method is described for separating plutonium from uranium and fission products by treating a nitrate solution of fission products, uranium, and hexavalent plutonium with a relatively water-insoluble fluoride to adsorb fission products on the fluoride, treating the residual solution with a reducing agent for plutonium to reduce its valence to four and less, treating the reduced plutonium solution with a relatively insoluble fluoride to adsorb the plutonium on the fluoride, removing the solution, and subsequently treating the fluoride with its adsorbed plutonium with a concentrated aqueous solution of at least one of a group consisting of aluminum nitrate, ferric nitrate, and manganous nitrate to remove the plutonium from the fluoride.

  6. Single crystal growth, superconductivity and Fermi surface study of plutonium compounds

    Energy Technology Data Exchange (ETDEWEB)

    Haga, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan)], E-mail: haga.yoshinori@jaea.go.jp; Aoki, D. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Yamagami, H. [Department of Physics, Faculty of Science, Kyoto Sangyo University, Kyoto 603-8555 (Japan); Matsuda, T.D. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Nakajima, K.; Arai, Y. [Nuclear Science and Engineering Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Yamamoto, E.; Nakamura, A. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Homma, Y. [Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Shiokawa, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Institute for Materials Research, Tohoku University, Oarai, Ibaraki 311-1313 (Japan); Onuki, Y. [Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195 (Japan); Graduate School of Science, Osaka University, Toyonaka, Osaka 560-0043 (Japan)

    2007-10-11

    Single crystals of plutonium compounds PuRhGa{sub 5} and PuIn{sub 3} are successfully grown. For PuRhGa{sub 5}, anisotropy of the superconducting upper critical field was found and analyzed by the anisotropic mass model, consistent with quasi-two-dimensional electronic states predicted by band calculations. On the other hand, the de Haas-van Alphen oscillation was observed in PuIn{sub 3}. By comparing with the band calculations, it is concluded that 5f electrons are itinerant in PuIn{sub 3}.

  7. Fractionation of plutonium in environmental and bio-shielding concrete samples using dynamic sequential extraction

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin

    2010-01-01

    Fractionation of plutonium isotopes (238Pu, 239,240Pu) in environmental samples (i.e. soil and sediment) and bio-shielding concrete from decommissioning of nuclear reactor were carried out by dynamic sequential extraction using an on-line sequential injection (SI) system combined with a specially...... designed extraction column. Plutonium in the fractions from the sequential extraction was separated by ion exchange chromatography and measured using alpha spectrometry. The analytical results show a higher mobility of plutonium in bio-shielding concrete, which means attention should be paid...

  8. Observations of surface-mediated reduction of Pu(VI) to Pu(IV) on hematite nanoparticles by ATR FT-IR

    Energy Technology Data Exchange (ETDEWEB)

    Emerson, Hilary P. [Florida International Univ., Applied Research Center, Miami, FL (United States); Powell, Brian A. [Clemson Univ., Dept. of Enviromental Engineering and Earth Sciences, Anderson, SC (United States)

    2015-07-01

    Previous studies have shown that mineral surfaces may facilitate the reduction of plutonium though the mechanisms of the reduction are still unknown. The objective of this study is to use batch sorption and attenuated total reflectance Fourier transform infrared spectroscopy experiments to observe the surface-mediated reduction of plutonium on hematite nanoparticles. These techniques allow for in situ measurement of reduction of plutonium with time and may lead to a better understanding of the mechanisms of surface mediated reduction of plutonium. For the first time, ATR FT-IR peaks for Pu(VI) sorbed to hematite are measured at ∝ 916 cm{sup -1}, respectively. The decrease in peak intensity with time provides a real-time, direct measurement of Pu(VI) reduction on the hematite surface. In this work pseudo first order rate constants estimated at the high loadings (22 mg{sub Pu}/g{sub hematite}, 1.34 x 10{sup -6} M{sub Pu}/m{sup 2}) for ATR FT-IR are approximately 10 x slower than at trace concentrations based on previous work. It is proposed that the reduced rate constant at higher Pu loadings occurs after the reduction capacity due to trace Fe(II) has been exhausted and is dependent on the oxidation of water and possibly electron shuttling based on the semiconducting nature of hematite. Therefore, the reduction rate at higher loadings is possibly due to the thermodynamic favorability of Pu(IV)-hydroxide complexes.

  9. MA Doping Analysis on Breeding Capability and Protected Plutonium Production of Large FBR

    Science.gov (United States)

    Permana, Sidik; Suzuki, Mitsutoshi; Kuno, Yusuke

    2010-06-01

    Spent fuel from LWR can be seen as long-live waste if it is not recycled or as a "new fuel" resource if it is recycled into the reactors. Uranium and plutonium have been used for "new fuel" resources from LWR spent fuel as MOX fuel type which is loaded into thermal reactor or fast reactor types. Other actinides from the spent fuel such as neptunium, americium and curium as minor actinide (MA) are considered to be loaded into the reactors for specific purposes, recently. Those purposes such as for increasing protected plutonium production and breeding capability for protected plutonium as well as in the same time those amount of MA can be reduced to a small quantity as a burner or transmutation purpose. Some investigations and scientific approaches are performed in order to increase a material "barrier" in plutonium isotope composition by increasing the even mass number of plutonium isotope such as Pu-238, Pu-240 and Pu-242 as plutonium protected composition. Higher material barrier which related to intrinsic properties of plutonium isotopes with even mass number (Pu-238, Pu-240 and Pu-242), are recognized because of their intense decay heat (DH) and high spontaneous fission neutron (SFN) rates. Those even number mass of plutonium isotope contribute to some criteria of plutonium characterization which will be adopted for present study such as IAEA, Pellaud and Kessler criteria (IAEA, 1972; Pellaud, 2002; and Kessler, 2007). The present paper intends to evaluate the breeding capability as a fuel sustainability index of the reactors and to analyze the composition of protected plutonium production of large power reactor based on the FaCT FBR as reference (Ohki, et al., 2008). Three dimensional FBR core configuration has been adopted which is based on the core optimization calculation of SRAC-CITATION code as reactor core analysis and JENDL-3.3 is adopted for nuclear data library. Some MA doping materials are loaded into the blanket regions which can be considered as

  10. Ostwald Ripening and Its Effect on PuO2 Particle Size in Hanford Tank Waste

    Energy Technology Data Exchange (ETDEWEB)

    Delegard, Calvin H.

    2011-09-29

    Between 1944 and 1989, the Hanford Site produced 60 percent (54.5 metric tons) of the United States weapons plutonium and produced an additional 12.9 metric tons of fuels-grade plutonium. High activity wastes, including plutonium lost from the separations processes used to isolate the plutonium, were discharged to underground storage tanks during these operations. Plutonium in the Hanford tank farms is estimated to be {approx}700 kg but may be up to {approx}1000 kg. Despite these apparent large quantities, the average plutonium concentration in the {approx}200 million liter tank waste volume is only about 0.003 grams per liter ({approx}0.0002 wt%). The plutonium is largely associated with low solubility metal hydroxide/oxide sludges where its low concentration and intimate mixture with neutron-absorbing elements (e.g., iron) are credited in nuclear criticality safety. However, concerns have been expressed that plutonium, in the form of plutonium hydrous oxide, PuO{sub 2} {center_dot} xH{sub 2}O, could undergo sufficient crystal growth through Ostwald ripening in the alkaline tank waste to potentially be separable from neutron absorbing constituents by settling or sedimentation. It was found that plutonium that entered the alkaline tank waste by precipitation through neutralization from acid solution is initially present as 2- to 3-nm (0.002- to 0.003-{mu}m) scale PuO{sub 2} {center_dot} xH{sub 2}O crystallite particles and grows from that point at exceedingly slow rates, posing no risk to physical segregation. These conclusions are reached by both general considerations of Ostwald ripening and specific observations of the behaviors of PuO{sub 2} and PuO{sub 2} {center_dot} xH{sub 2}O upon aging in alkaline solution.

  11. FY12 Final Report for PL10-Mod Separations-PD12: Electrochemically Modulated Separation of Plutonium from Dilute and Concentrated Dissolver Solutions for Analysis by Gamma Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Pratt, Sandra H.; Arrigo, Leah M.; Duckworth, Douglas C.; Cloutier, Janet M.; Breshears, Andrew T.; Schwantes, Jon M.

    2013-05-01

    Accurate and timely analysis of plutonium in spent nuclear fuel is critical in nuclear safeguards for detection of both protracted and rapid plutonium diversions. Gamma spectroscopy is a viable method for accurate and timely measurements of plutonium provided that the plutonium is well separated from the interfering fission and activation products present in spent nuclear fuel. Electrochemically modulated separation (EMS) is a method that has been used successfully to isolate picogram amounts of Pu from nitric acid matrices. With EMS, Pu adsorption may be turned “on” and “off” depending on the applied voltage, allowing for collection and stripping of Pu without the addition of chemical reagents. In this work, we have scaled up the EMS process to isolate microgram quantities of Pu from matrices encountered in spent nuclear fuel during reprocessing. Several challenges have been addressed including surface area limitations, radiolysis effects, electrochemical cell performance stability, and chemical interferences. After these challenges were resolved, 6 µg Pu was deposited in the electrochemical cell with approximately an 800-fold reduction of fission and activation product levels from a spent nuclear fuel sample. Modeling showed that these levels of Pu collection and interference reduction may not be sufficient for Pu detection by gamma spectroscopy. The main remaining challenges are to achieve a more complete Pu isolation and to deposit larger quantities of Pu for successful gamma analysis of Pu. If gamma analyses of Pu are successful, EMS will allow for accurate and timely on-site analysis for enhanced Pu safeguards.

  12. Novel insights into Fukushima nuclear accident from isotopic evidence of plutonium spread along coastal rivers.

    Science.gov (United States)

    Evrard, Olivier; Pointurier, Fabien; Onda, Yuichi; Chartin, Caroline; Hubert, Amélie; Lepage, Hugo; Pottin, Anne-Claire; Lefèvre, Irène; Bonté, Philippe; Laceby, J Patrick; Ayrault, Sophie

    2014-08-19

    The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

  13. Reduction of Tetravalent Plutonium in the Presence of Acetohydroxamic Acid

    Energy Technology Data Exchange (ETDEWEB)

    Tkac, Peter [Radiation Center, Oregon State University, Corvallis, OR (United States); Precek, Martin [Department of Chemistry, Oregon State University, Corvallis, OR (United States); Paulenova, Alena [Department of Nuclear Engineering and Radiation Health Physics, Oregon State University, Corvallis, OR (United States)

    2009-06-15

    Acetohydroxamic acid (AHA) has been proposed as a salt-free stripping reagent in the modified PUREX process for the spent nuclear fuel re-processing. AHA is a capable reductant of Np(VI) and Pu(VI) and a strong complexant for tetravalent neptunium and plutonium; hence, its behavior must be studied in detail. For better characterization of the all relevant chemical processes and successful design of the future separation flowsheets it is important to predict the speciation and partitioning of Pu between the organic and aqueous phases in the proposed extraction systems containing acetohydroxamic acid. The hydrolytic instability of hydroxamic group under acidic conditions causes a slow degradation of AHA followed by formation of acetic acid and hydroxylamine which also acts as a reductant of Pu(IV). The complexes of Pu(IV) with AHA are very strong; however, under acidic conditions, the chelate ring prevents the acidic hydrolysis only temporarily. The decomposition of Pu-aceto-hydroxamate complex and reduction of Pu(IV) to Pu(III) observed for these systems was investigated in the present paper. Reduction of Pu(IV) in the presence of AHA was monitored by Vis-NIR spectroscopy in the range of 400-700 nm. All complexes between Pu(IV) and AHA have a very intense absorption in this region; therefore, for a better resolution of spectra, all experiments were performed under low AHA:Pu ratios, where only two species, non-complexed Pu(IV) and Pu(IV)-mono-aceto-hydroxamate complex, are initially present in relevant concentrations. To characterize the rate and the reaction mechanism, spectra were collected as a function of time for different initial concentrations of reactants and analyzed at several wavelengths using the data on extinction coefficients for all absorbing species. The extinction coefficient for Pu(IV)-AHA complex was resolved by fitting the absorption spectra with the chemical equilibrium modeling software FITEQL 4.0. The analysis of the experimental data obtained

  14. Equilibrium composition for the reaction of plutonium hydride with air

    Institute of Scientific and Technical Information of China (English)

    2002-01-01

    There are six independent constituents with 4 chemical elements, i.e. PuH2.7(s), PuN(s), Pu2O3(s), N2, O2 and H2, therefore , the system described involves of 2 independent reactions ,both those of the experimental, which indicates that the chemical equilibrium is nearly completely approached. Therefore, it is believed that the reaction rate of plutonium hydride with air is extremely rapid. The present paper has briefly discussed the simultaneous reactions and its thermodynamic coupling effect.

  15. 242Pu as tracer for simultaneous determination of 237Np and 239,240Pu in environmental samples

    DEFF Research Database (Denmark)

    Chen, Q.J.; Dahlgaard, H.; Nielsen, S.P.;

    2002-01-01

    A procedure has been developed using Pu-242 as tracer for simultaneous determination of Np-237 and Pu-239,Pu-240 in environmental samples. The validity of the method has been demonstrated by ICPMS and alpha-spectroscopy for up to 10 gram soil and sediment, seawater up to 200 litres. The paper...... describes a suitable chemical procedure for Np and Pu including a quantitative pre-concentration of neptunium and plutonium, preparation of Np4+ and Pu4+, NP(NO3)(6)(2-) and Pu(NO3)(6)(2-), The ratio of Np-237/Pu-242 (or Np-237/Pu-239) before and after the procedure has been determined using 10 g soil (free...... from Np and Pu) R-before/R-after = 1.004 +/- 3.3% (S.D n = 20) and 1 litre seawater R-before/R-after = 1.019+/-1.9% (S.D., n = 12). Results from the intercomparison samples LAEA-135, LAEA-381 and from environmental samples are presented....

  16. FORM AND AGING OF PLUTONIUM IN SAVANNAH RIVER SITE WASTE TANK 18

    Energy Technology Data Exchange (ETDEWEB)

    Hobbs, D.

    2012-02-24

    This report provides a summary of the effects of aging on and the expected forms of plutonium in Tank 18 waste residues. The findings are based on available information on the operational history of Tank 18, reported analytical results for samples taken from Tank 18, and the available scientific literature for plutonium under alkaline conditions. These findings should apply in general to residues in other waste tanks. However, the operational history of other waste tanks should be evaluated for specific conditions and unique operations (e.g., acid cleaning with oxalic acid) that could alter the form of plutonium in heel residues. Based on the operational history of other tanks, characterization of samples from the heel residues in those tanks would be appropriate to confirm the form of plutonium. During the operational period and continuing with the residual heel removal periods, Pu(IV) is the dominant oxidation state of the plutonium. Small fractions of Pu(V) and Pu(VI) could be present as the result of the presence of water and the result of reactions with oxygen in air and products from the radiolysis of water. However, the presence of Pu(V) would be transitory as it is not stable at the dilute alkaline conditions that currently exists in Tank 18. Most of the plutonium that enters Savannah River Site (SRS) high-level waste (HLW) tanks is freshly precipitated as amorphous plutonium hydroxide, Pu(OH){sub 4(am)} or hydrous plutonium oxide, PuO{sub 2(am,hyd)} and coprecipitated within a mixture of hydrous metal oxide phases containing metals such as iron, aluminum, manganese and uranium. The coprecipitated plutonium would include Pu{sup 4+} that has been substituted for other metal ions in crystal lattice sites, Pu{sup 4+} occluded within hydrous metal oxide particles and Pu{sup 4+} adsorbed onto the surface of hydrous metal oxide particles. The adsorbed plutonium could include both inner sphere coordination and outer sphere coordination of the plutonium. PuO{sub 2

  17. Standard test method for plutonium by Iron (II)/Chromium (VI) amperometric titration

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2002-01-01

    1.1 This test method covers the determination of plutonium in unirradiated nuclear-grade plutonium dioxide, uranium-plutonium mixed oxides with uranium (U)/plutonium (Pu) ratios up to 21, plutonium metal, and plutonium nitrate solutions. Optimum quantities of plutonium to measure are 7 to 15 mg. 1.2 The values stated in SI units are to be regarded as standard. No other units of measurement are included in this standard. 1.3 This standard does not purport to address all of the safety concerns, if any, associated with its use. It is the responsibility of the user of this standard to establish appropriate safety and health practices and determine the applicability of regulatory limitations prior to use.

  18. Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations.

    Science.gov (United States)

    Schneider, Stephanie; Walther, Clemens; Bister, Stefan; Schauer, Viktoria; Christl, Marcus; Synal, Hans-Arno; Shozugawa, Katsumi; Steinhauser, Georg

    2013-10-18

    The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio ²⁴⁰Pu/²³⁹Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 ± 0.046) evidences that the Pu originates from a nuclear reactor (²³⁹⁺²⁴⁰Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated.

  19. Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope

    Science.gov (United States)

    Armstrong, Christopher R.; Brant, Heather A.; Nuessle, Patterson R.; Hall, Gregory; Cadieux, James R.

    2016-01-01

    Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., 244Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic 244Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken at SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Significant 244Pu was measured in all of the years sampled with the highest amount observed in 2003. The 244Pu content, in femtograms (fg = 10−15 g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the 244Pu/239Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively. PMID:26898531

  20. Determination of Pu in soil samples; Determinacion de Pu en muestras de suelo

    Energy Technology Data Exchange (ETDEWEB)

    Torres C, C. O.; Hernandez M, H.; Romero G, E. T. [ININ, Carretera Mexico-Toluca s/n, 52750 Ocoyoacac, Estado de Mexico (Mexico); Vega C, H. R., E-mail: carioli_32907@hotmail.com [Universidad Autonoma de Zacatecas, Unidad Academica de Estudios Nucleares, Cipres No. 10, Fracc. La Penuela, 98068 Zacatecas, Zac. (Mexico)

    2016-10-15

    The irreversible consequences of accidents occurring in nuclear plants and in nuclear fuel reprocessing sites are mainly the distribution of different radionuclides in different matrices such as the soil. The distribution in the superficial soil is related to the internal and external exposure to the radiation of the affected population. The internal contamination with radionuclides such as Pu is of great relevance to the nuclear forensic science, where is important to know the chemical and isotopic compositions of nuclear materials. The objective of this work is to optimize the radiochemical separation of plutonium (Pu) from soil samples and to determine their concentration. The soil samples were prepared using acid digestion assisted by microwave; purification of Pu was carried out with AG1X8 resin using ion exchange chromatography. Pu isotopes were measured using ICP-SFMS. In order to reduce the interference due to the presence of {sup 238}UH {sup +} in the samples, a solvent removal system (Apex) was used. In addition, the limit of detection and quantification of Pu was determined. It was found that the recovery efficiency of Pu in soil samples ranges from 70 to 93%. (Author)

  1. Plutonium Consumption Program, CANDU Reactor Project final report

    Energy Technology Data Exchange (ETDEWEB)

    1994-07-31

    DOE is investigating methods for long term dispositioning of weapons grade plutonium. One such method would be to utilize the plutonium in Mixed OXide (MOX) fuel assemblies in existing CANDU reactors. CANDU (Canadian Deuterium Uranium) reactors are designed, licensed, built, and supported by Atomic Energy of Canada Limited (AECL), and currently use natural uranium oxide as fuel. The MOX spent fuel assemblies removed from the reactor would be similar to the spent fuel currently produced using natural uranium fuel, thus rendering the plutonium as unattractive as that in the stockpiles of commercial spent fuel. This report presents the results of a study sponsored by the DOE for dispositioning the plutonium using CANDU technology. Ontario Hydro`s Bruce A was used as reference. The fuel design study defined the optimum parameters to disposition 50 tons of Pu in 25 years (or 100 tons). Two alternate fuel designs were studied. Safeguards, security, environment, safety, health, economics, etc. were considered. Options for complete destruction of the Pu were also studied briefly; CANDU has a superior ability for this. Alternative deployment options were explored and the potential impact on Pu dispositioning in the former Soviet Union was studied. An integrated system can be ready to begin Pu consumption in 4 years, with no changes required to the reactors other than for safe, secure storage of new fuel.

  2. Further Studies of Plutonium and Americium at Thule, Greenland

    DEFF Research Database (Denmark)

    Aarkrog, Asker; Dahlgaard, Henning; Nilsson, Karen Kristina

    1984-01-01

    Eleven years after the accidental loss of nuclear weapons in 1968, the fourth scientific expedition to Thule occurred. The estimated inventory of 1 TBq 239,240Pu in the marine sediments was unchanged when compared with the estimate based on the 1974 data. Plutonium from the accident had moved fur...

  3. System specification for the plutonium stabilization and packaging system

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1996-07-01

    This document describes functional design requirements for the Plutonium Stabilization and Packaging System (Pu SPS), as required by DOE contract DE-AC03-96SF20948 through contract modification 9 for equipment in Building 707 at Rocky Flats Environmental Technology Site (RFETS).

  4. Separation Method of Neptunium From Large Amount of Plutonium

    Institute of Scientific and Technical Information of China (English)

    JIN; Hua; SU; Yu-lan; YING; Zhe-cong; ZHAO; Sheng-yang

    2013-01-01

    A new separation method of neptunium from large amount of plutonium by TEVA column has been developed.A series of influence factors are studied such as resin’s types,valence adjusting of Np and Pu,extraction and elution behavior of Np on TEVA resin.According to above works,a separation procedure is recommended as follows:1)Adjusting the

  5. ARRAYS OF BOTTLES OF PLUTONIUM NITRATE SOLUTION

    Energy Technology Data Exchange (ETDEWEB)

    Margaret A. Marshall

    2012-09-01

    In October and November of 1981 thirteen approaches-to-critical were performed on a remote split table machine (RSTM) in the Critical Mass Laboratory of Pacific Northwest Laboratory (PNL) in Richland, Washington using planar arrays of polyethylene bottles filled with plutonium (Pu) nitrate solution. Arrays of up to sixteen bottles were used to measure the critical number of bottles and critical array spacing with a tight fitting Plexiglas® reflector on all sides of the arrays except the top. Some experiments used Plexiglas shells fitted around each bottles to determine the effect of moderation on criticality. Each bottle contained approximately 2.4 L of Pu(NO3)4 solution with a Pu content of 105 g Pu/L and a free acid molarity H+ of 5.1. The plutonium was of low 240Pu (2.9 wt.%) content. These experiments were sponsored by Rockwell Hanford Operations because of the lack of experimental data on the criticality of arrays of bottles of Pu solution such as might be found in storage and handling at the Purex Facility at Hanford. The results of these experiments were used “to provide benchmark data to validate calculational codes used in criticality safety assessments of [the] plant configurations” (Ref. 1). Data for this evaluation were collected from the published report (Ref. 1), the approach to critical logbook, the experimenter’s logbook, and communication with the primary experimenter, B. Michael Durst. Of the 13 experiments preformed 10 were evaluated. One of the experiments was not evaluated because it had been thrown out by the experimenter, one was not evaluated because it was a repeat of another experiment and the third was not evaluated because it reported the critical number of bottles as being greater than 25. Seven of the thirteen evaluated experiments were determined to be acceptable benchmark experiments. A similar experiment using uranyl nitrate was benchmarked as U233-SOL-THERM-014.

  6. Radiochemical Separation and Measurement by Mass Spectrometry with Magnetic Sector with Inductively Coupled Plasma source (ICP-SFMS of Plutonium Isotopes in Soil Samples

    Directory of Open Access Journals (Sweden)

    C. O. Torres-Cortés

    2016-08-01

    Full Text Available The aim of this work is twofold: to optimize the radiochemical separation of Plutonium (Pu from soil samples, and to measure the Pu concentration. Soil samples were prepared using acid digestion assisted by microwaves; then, Pu purification was carried out with Pu AG1X8 resin. Pu isotopes were measured using Mass Spectrometry with Magnetic Sector with Inductively Coupled Plasma source (ICP-SFMS. In order to reduce the interference due to the presence of 238UH+ in the samples a desolvation system (Apex was used. The limit of detection (LOD of Pu was determined. The efficiency of Pu recovery from soil samples varies from 70 to 93%.

  7. Radiative capture on $^{242}$Pu for MOX fuel reactors

    CERN Multimedia

    The use of MOX fuel (mixed-oxide fuel made of UO$_{2}$ and PuO$_{2}$) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. Indeed around 66% of the plutonium from spent fuel is made of $^{239}$Pu and $^{241}$Pu, which are fissile in thermal reactors. A typical reactor of this type uses a fuel with 7% reprocessed Pu and 93% depleted U, thus profiting from both the spent fuel and the remaining $^{238}$U following the $^{235}$U enrichment. With the use of such new fuel compositions rich in Pu the better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. This is clearly stated in the recent OECD NEA’s “High Priority Request List” and in the WPEC-26 “Uncertainty and target accuracy assessment for innovative systems using recent covariance data evaluations” report. In particular, a new series of cross section evaluations have been recently carried out jointly by the European (JEFF) and United ...

  8. Plutonium in the marine environment at Thule, NW-Greenland after a nuclear weapons accident

    DEFF Research Database (Denmark)

    Dahlgaard, H.; Eriksson, M.; Ilus, E.

    2001-01-01

    In January 1968, a B52 plane carrying 4 nuclear weapon!: crashed on the sea ice similar to 12 km from the Thule Air Base, in northwest Greenland. The benthic marine environment in the 180-230 m deep Bylot Sound was then contaminated with similar to1.4 TBq Pu-239,Pu-240 (similar to0.5 kg). The site...... than in sediments. Some biota groups show a somewhat higher uptake of americium than of plutonium. Sediment samples with weapons plutonium from the accident show a significant variation in Pu-240/Pu-239 atom ratios in the range 0.027-0.057. This supports the hypothesis that the Thule plutonium...

  9. Transfer of plutonium to rat embryos in vivo and in vitro

    Energy Technology Data Exchange (ETDEWEB)

    Takahashi, Sentaro; Sato, Hiroshi; Kubota, Yoshihisa; Inaba, Jiro (National Inst. of Radiological Sciences, Chiba (Japan))

    1992-12-01

    The [sup 239]Pu distribution in the 12.5-day-old rat conceptus was compared between in vivo and in vitro experimental systems to establish a possible mechanism of cross-palcental transfer of this radionuclide. In the in vivo study, plutonium citrate solution was injected intravenously to pregnant Wistar rats. In the in vitro study, either plutonium citrate or plutonium hydroxide colloid was administered, as a solution of Eagle MEM and FCS containing [sup 239]Pu at the concentration used in the maternal serum in the in vivo experiments, to rat conceptuses maintained by the whole-embryo culture method. The concentration of [sup 239]Pu in the yolk sac ([sup 239]Pu activity per gram wet weight) were much higher than in the embryo in both the in vivo and in vitro experiments, suggesting that the yolk sac may be an effective barrier against the transfer of plutonium to the embryos. The ratios of the [sup 239]Pu concentration in the yolk sac to that in the embryo were relatively constant with time after administration in the in vitro system; 18-27 for plutonium citrate and 67-84 for plutonium hydroxide. In the in vivo experiment, these ratios changed with time after injection; 15 at 5 min and 62 and 60 min after injection. This suggests that in the in vivo system, the chemical form of [sup 239]Pu changed with time after injection, probably to a macromolecular form such as the hydroxide colloid or plutonium-protein complex although [sup 239]Pu was injected to the maternal blood as citrate. (author).

  10. Plutonium isotopes in the ocean off Japan after Fukushima

    Energy Technology Data Exchange (ETDEWEB)

    Buesseler, K.; Black, E.; Pike, S. [Woods Hole Oceanographic Institution (United States); Kenna, T. [Lamont-Doherty Earth Observatory (United States); Masque, P. [Universitat Autonoma de Barcelona (Spain)

    2014-07-01

    The Fukushima Dai-ichi nuclear power plants (NPPs) are known to be an unprecedented accidental source of {sup 137}Cs, {sup 134}Cs and other volatile radionuclides to the ocean. Much less is known however about the extent of input of refractory radionuclides such as plutonium to the environment. Limited available data from land soils and vegetation, suggest at least some atmospheric delivery of particulate Pu but at very low levels relative to pre-existing fallout sources. To resolve Fukushima derived Pu from weapons testing derived Pu, information regarding the Pu isotopic composition is needed. The {sup 240}Pu/{sup 239}Pu atom ratio determined by mass spectrometric techniques, and the {sup 238}Pu/{sup 239,240}Pu activity ratio as measured by alpha counting are diagnostic with respect to Pu source. We review and present new data on the Pu isotopic ratios and concentrations in the oceans, combining several data sets on dissolved (from bottle sampling), suspended particulates (from filtration), sinking particles (from sediment traps) and seafloor sediments (from cores) to look for the Fukushima Pu signal. In most samples, the {sup 240}Pu/{sup 239}Pu ratios are in the range of 0.20-0.23, characteristic of Pu ocean signal which is a combination of global fallout with a characteristic ratio of 0.18 and local fallout from the Pacific Proving Grounds with ratios higher than 0.24, and known from prior studies to influence the ocean off Japan. In 2011, in surface ocean waters, we found ratios {sup 240}Pu/{sup 239}Pu >0.3, which implies a component of Fukushima Pu had been delivered to the ocean, given NPP derived end-member ratios of 0.35-0.45. Fukushima derived Pu was not found deeper in the water column or even at all stations, consistent with its rapid removal from the ocean and the high background of pre-existing Pu in the waters and sediments, masking the new Fukushima sources. With this data a mass balance will be made between Pu from global fallout, local fallout and

  11. Speciation and Bioavailability Measurements of Environmental Plutonium Using Diffusion in Thin Films.

    Science.gov (United States)

    Cusnir, Ruslan; Steinmann, Philipp; Christl, Marcus; Bochud, François; Froidevaux, Pascal

    2015-11-09

    The biological uptake of plutonium (Pu) in aquatic ecosystems is of particular concern since it is an alpha-particle emitter with long half-life which can potentially contribute to the exposure of biota and humans. The diffusive gradients in thin films technique is introduced here for in-situ measurements of Pu bioavailability and speciation. A diffusion cell constructed for laboratory experiments with Pu and the newly developed protocol make it possible to simulate the environmental behavior of Pu in model solutions of various chemical compositions. Adjustment of the oxidation states to Pu(IV) and Pu(V) described in this protocol is essential in order to investigate the complex redox chemistry of plutonium in the environment. The calibration of this technique and the results obtained in the laboratory experiments enable to develop a specific DGT device for in-situ Pu measurements in freshwaters. Accelerator-based mass-spectrometry measurements of Pu accumulated by DGTs in a karst spring allowed determining the bioavailability of Pu in a mineral freshwater environment. Application of this protocol for Pu measurements using DGT devices has a large potential to improve our understanding of the speciation and the biological transfer of Pu in aquatic ecosystems.

  12. Evidence of plutonium bioavailability in pristine freshwaters of a karst system of the Swiss Jura Mountains

    Science.gov (United States)

    Cusnir, Ruslan; Christl, Marcus; Steinmann, Philipp; Bochud, François; Froidevaux, Pascal

    2017-06-01

    The interaction of trace environmental plutonium with dissolved natural organic matter (NOM) plays an important role on its mobility and bioavailability in freshwater environments. Here we explore the speciation and biogeochemical behavior of Pu in freshwaters of the karst system in the Swiss Jura Mountains. Chemical extraction and ultrafiltration methods were complemented by diffusive gradients in thin films technique (DGT) to measure the dissolved and bioavailable Pu fraction in water. Accelerator mass spectrometry (AMS) was used to accurately determine Pu in this pristine environment. Selective adsorption of Pu (III, IV) on silica gel showed that 88% of Pu in the mineral water is found in +V oxidation state, possibly in a highly soluble [PuO2+(CO3)n]m- form. Ultrafiltration experiments at 10 kDa yielded a similar fraction of colloid-bound Pu in the organic-rich and in mineral water (18-25%). We also found that the concentrations of Pu measured by DGT in mineral water are similar to the bulk concentration, suggesting that dissolved Pu is readily available for biouptake. Sequential elution (SE) of Pu from aquatic plants revealed important co-precipitation of potentially labile Pu (60-75%) with calcite fraction within outer compartment of the plants. Hence, we suggest that plutonium is fully available for biological uptake in both mineral and organic-rich karstic freshwaters.

  13. Hybrid density functional study on lattice vibration, thermodynamic properties, and chemical bonding of plutonium monocarbide

    Science.gov (United States)

    Rong, Yang; Bin, Tang; Tao, Gao; BingYun, Ao

    2016-06-01

    Hybrid density functional theory is employed to systematically investigate the structural, magnetic, vibrational, thermodynamic properties of plutonium monocarbide (PuC and PuC0.75). For comparison, the results obtained by DFT, DFT + U are also given. For PuC and PuC0.75, Fock-0.25 hybrid functional gives the best lattice constants and predicts the correct ground states of antiferromagnetic (AFM) structure. The calculated phonon spectra suggest that PuC and PuC0.75 are dynamically stable. Values of the Helmholtz free energy ΔF, internal energy ΔE, entropy S, and constant-volume specific heat C v of PuC and PuC0.75 are given. The results are in good agreement with available experimental or theoretical data. As for the chemical bonding nature, the difference charge densities, the partial densities of states and the Bader charge analysis suggest that the Pu-C bonds of PuC and PuC0.75 have a mixture of covalent character and ionic character. The effect of carbon vacancy on the chemical bonding is also discussed in detail. We expect that our study can provide some useful reference for further experimental research on the phonon density of states, thermodynamic properties of the plutonium monocarbide. Project supported by the National Natural Science Foundation of China (Grant Nos. 21371160 and 21401173).

  14. High Surplus Means High Profits?

    Institute of Scientific and Technical Information of China (English)

    Guo Yan

    2007-01-01

    @@ In recent years,China has been in the limelight worldwide due to its constant high trade surplus.Its trade surplus hit US$ 24.974 billion in August, a record high and an increase of US$ 624 million versus the previous month, according to the latest data from China Customs.

  15. Ab initio equation-of-state and elastic properties of Pu metal and Pu-Ga alloys

    Science.gov (United States)

    Per, Soderlind; Landa, Alex

    2010-03-01

    We present results of ab initio calculations of equation-of-state and elastic properties for Pu metal and Pu-Ga alloys. For this we have employed density-functional theory (DFT) in conjunction with spin-orbit coupling and orbital polarization for the metal and coherent-potential approximation (CPA) for the alloys. All Pu systems benefit from spin polarization which is consistent with previous DFT studies of plutonium. We show that orbital correlations become more important proceeding from α->β->γ plutonium, thus suggesting increasing f-electron correlation (localization). For δ-Pu- Ga alloys we find that the system softens with larger Ga content, i.e., bulk modulus, elastic constants, and chemical bonding weakens with increasing Ga concentration. This inverse relationship is nearly linear and supported by measurements on polycrystal δ-Pu-Ga alloys. For Pu metal, our single-crystal results also relates reasonably with ultrasound data on polycrystal samples where available. The comparison is indirect but made possible by approximating the polycrystal with an isotropic (uniform strain) single crystal. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

  16. Determination of filter pore size for use in HB line phase II production of plutonium oxide

    Energy Technology Data Exchange (ETDEWEB)

    Shehee, T. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Crowder, M. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Rudisill, T. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2014-08-01

    H-Canyon and HB-Line are tasked with the production of plutonium oxide (PuO2) from a feed of plutonium (Pu) metal. The PuO2 will provide feed material for the Mixed Oxide (MOX) Fuel Fabrication Facility. After dissolution of the Pu metal in H-Canyon, plans are to transfer the solution to HB-Line for purification by anion exchange. Anion exchange will be followed by plutonium(IV) oxalate precipitation, filtration, and calcination to form PuO2. The filtrate solutions, remaining after precipitation, contain low levels of Pu ions, oxalate ions, and may include solids. These solutions are transferred to H-Canyon for disposition. To mitigate the criticality concern of Pu solids in a Canyon tank, past processes have used oxalate destruction or have pre-filled the Canyon tank with a neutron poison. The installation of a filter on the process lines from the HB-Line filtrate tanks to H-Canyon Tank 9.6 is proposed to remove plutonium oxalate solids. This report describes SRNL’s efforts to determine the appropriate pore size for the filters needed to perform this function. Information provided in this report aids in developing the control strategies for solids in the process.

  17. Interaction of aerobic soil bacteria with plutonium(VI)

    Energy Technology Data Exchange (ETDEWEB)

    Panak, P.J. [Lawrence Berkeley National Lab., Berkeley, CA (United States). Chemical Sciences Div.; Nitsche, H. [Lawrence Berkeley National Lab., Berkeley, CA (United States). Chemical Sciences Div.; California Univ., Berkeley, CA (United States). Dept. of Chemistry

    2001-07-01

    We studied the interaction of Pu(VI) with Pseudomonas stutzeri ATCC 17588 and Bacillus sphaericus ATCC 14577, representatives of the main aerobic groups of soil bacteria present in the upper soil layers. The biosorption studies have shown that these soil bacteria accumulate high amounts of Pu(VI). The relative sorption efficiency toward Pu(VI) related to the amount of biomass used decreased with increasing biomass concentration due to increased agglomeration of the bacteria resulting in a decrease of the number of available complexing groups. Spores of Bacillus sphaericus showed a higher biosorption than the vegetative cells at low biomass concentration which decreased significantly with increasing biomass concentration. At higher biomass concentrations (> 0.7 g/L), the vegetative cells of both strains and the spores of B. sphaericus showed comparable sorption efficiencies. Investigations on the pH dependency of the biosorption and extraction studies with 0.01 M EDTA solution have shown that the biosorption of plutonium is a reversible process and the plutonium is bound by surface complexation. Optical absorption spectroscopy showed that one third of the initially present Pu(VI) was reduced to Pu(V) after 24 hours. Kinetic studies and solvent extraction to separate different oxidation states of Pu after contact with the biomass provided further information on the yield and the kinetics of the bacteria-mediated reduction. Long-term studies showed that also 16% of Pu(IV) was formed after one month. The slow kinetics of this process indicate that under our experimental conditions the Pu(IV) was not a produced by microbial reduction but seemed to be rather the result of the disproportionation of the formed Pu(V) or autoreduction of Pu(VI). (orig.)

  18. Characterisation of the plutonium isotopic composition of a sediment core from Palomares, Spain, by low-energy AMS and alpha-spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Chamizo, E., E-mail: elechacal@alum.us.e [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Jimenez-Ramos, M.C.; Enamorado, S.M. [Centro Nacional de Aceleradores (CNA), Isla de la Cartuja, 41092 Seville (Spain); Garcia-Leon, M. [Departamento de Fisica Atomica, Molecular y Nuclear, Universidad de Sevilla, 41012 Sevilla (Spain); Garcia-Tenorio, R. [Departamento de Fisica Aplicada II, E.T.S.A, Universidad de Sevilla, 41012 Sevilla (Spain); Mas, J.L. [Departamento de Fisica Aplicada I, Universidad de Sevilla, 41012 Sevilla (Spain); Masque, P. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); Merino, J. [Amphos 21, Pg. de Rubi 29-31, E-08197 Valldoreix (Spain); Sanchez-Cabeza, J.A. [Institut de Ciencia i Tecnologia Ambientals, Department de Fisica, Universitat Autonoma de Barcelona, 08193 Bellaterra (Spain); International Atomic Energy Agency, Marine Environment Laboratories, MC-98000 (Monaco)

    2010-04-15

    The measurement of plutonium isotopes, {sup 239}Pu and {sup 240}Pu, at 670 kV on the compact accelerator mass spectrometry (AMS) system at the Centro Nacional de Aceleradores (CNA) in Seville, Spain, is now a reality. In this work, we present first Pu AMS results for environmental samples: a sediment core collected in a submarine canyon in the Mediterranean coast of the Spanish region of Palomares, affected by a nuclear accident in 1966. From the study of the {sup 240}Pu/{sup 239}Pu atomic ratio profile, showing on average levels lower than 11%, we confirm that the weapon-grade plutonium released on land during the accident, with a characteristic {sup 240}Pu/{sup 239}Pu atomic ratio of 5.8%, has found its way into the marine environment. A two-plutonium sources mixture model (Palomares and fallout) is used to elucidate the percentage of the plutonium coming from the accident. As a validation exercise of the Pu AMS measuring technique and in order to obtain the {sup 238}Pu/{sup (239+240)}Pu activity ratios, samples were also studied by alpha-spectrometry (AS). The obtained AS {sup 239+240}Pu activity concentration results fit in with the AMS ones in a wide dynamic range, thus validating the AMS technique.

  19. High-temperature vacuum distillation separation of plutonium waste salts

    Energy Technology Data Exchange (ETDEWEB)

    Garcia, E. [Los Alamos National Lab., NM (United States)

    1996-10-01

    In this task, high-temperature vacuum distillation separation is being developed for residue sodium chloride-potassium chloride salts resulting from past pyrochemical processing of plutonium. This process has the potential of providing clean separation of the salt and the actinides with minimal amounts of secondary waste generation. The process could produce chloride salt that could be discarded as low-level waste (LLW) or low actinide content transuranic (TRU) waste, and a concentrated actinide oxide powder that would meet long-term storage standards (DOE-DTD-3013-94) until a final disposition option for all surplus plutonium is chosen.

  20. Plutonium Finishing Plant

    Data.gov (United States)

    Federal Laboratory Consortium — The Plutonium Finishing Plant, also known as PFP, represented the end of the line (the final procedure) associated with plutonium production at Hanford.PFP was also...

  1. Plutonium Training Opportunities

    Energy Technology Data Exchange (ETDEWEB)

    Balatsky, Galya Ivanovna [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Wolkov, Benjamin [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-03-26

    This report was created to examine the current state of plutonium training in the United States and to discover ways in which to ensure that the next generation of plutonium workers are fully qualified.

  2. Determination of Pu-238 and Pu-239+240 in marine sediment samples of southern brazilian coast; Determinacao de Pu-238 e Pu-239+240 em amostras de sedimento marinho da costa sul brasileira

    Energy Technology Data Exchange (ETDEWEB)

    Figueira, Rubens C.L.; Cunha, Ieda Irma Lamas [Instituto de Pesquisas Energeticas e Nucleares (IPEN), Sao Paulo, SP (Brazil)]. E-mail: figueira@curiango.ipen.br; Furtado, Valdenir V.; Tessler, Moyses G. [Sao Paulo Univ., SP (Brazil). Inst. Oceanografico

    2000-07-01

    This work presents Pu-238 and Pu-239+240 levels from southern brazilian coast, in the region between Cabo de Santa Marta Grande (SC) and Cabo Frio (RJ), involving the seaside to external continental shelf. Pu-238 and Pu-239+240 levels in this region ranged from 15 to 150 mBq.kg{sup -1} and from 18.2 to 228 mBq.kg{sup -1}, respectively. The values are in agreement with the established range for south hemisphere as a result of the atmospheric fallout. The methodology for plutonium determination reached 30% to 75% as yield recovery and 4.2 mBq.kg{sup -1} as minimum detectable concentration (MDC). Thus the methodology is applicable to environmental samples analysis at low levels of the studied radionuclides. (author)

  3. [239Pu and chromosomal aberrations in human peripheral blood lymphocytes].

    Science.gov (United States)

    Okladnikova, N D; Osovets, S V; Kudriavtseva, T I

    2009-01-01

    The genome status in somatic cells was assessed using the chromosomal aberration (CA) test in peripheral blood lymphocytes from 194 plutonium workers exposed to occupational radiation mainly from low-transportable compounds of airborne 230Pu. Pu body burden at the time of cytogenetic study varied from values close to the method sensitivity to values multiply exceeding the permissible level. Standard (routine) methods of peripheral blood lymphocytes cultivation were applied. Chromatid- and chromosomal-type structural changes were estimated. Aberrations were estimated per 100 examined metaphase cells. The quantitative relationship between the CA frequency and Pu body burden and the absorbed dose to the lung was found. Mathematical processing of results was carried out based on the phenomenological model. The results were shown as theoretical and experimental curves. The threshold of the CA yield was 0.43 +/- 0.03 kBq (Pu body burden) and 6.12 +/- 1.20 cGy (absorbed dose to the lung).

  4. PLUTONIUM-THORIUM ALLOYS

    Science.gov (United States)

    Schonfeld, F.W.

    1959-09-15

    New plutonium-base binary alloys useful as liquid reactor fuel are described. The alloys consist of 50 to 98 at.% thorium with the remainder plutonium. The stated advantages of these alloys over unalloyed plutonium for reactor fuel use are easy fabrication, phase stability, and the accompanying advantuge of providing a means for converting Th/sup 232/ into U/sup 233/.

  5. PLUTONIUM CLEANING PROCESS

    Science.gov (United States)

    Kolodney, M.

    1959-12-01

    A method is described for rapidly removing iron, nickel, and zinc coatings from plutonium objects while simultaneously rendering the plutonium object passive. The method consists of immersing the coated plutonium object in an aqueous acid solution containing a substantial concentration of nitrate ions, such as fuming nitric acid.

  6. Refined data on the PuO{sub 4} volatility

    Energy Technology Data Exchange (ETDEWEB)

    Domanov, V.P.; Lobanov, Yu.V. [Joint Institute for Nuclear Research, Dubna (Russian Federation)

    2004-07-01

    In thermochromatographic (TC) studies on the thermal oxidation of trace quantities of plutonium in a stream of a He+O{sub 2} mixture, the formation of some volatile forms was observed. The most volatile compound was adsorbed on a quartz surface at a negative temperature of about -100 C. In the ref., we assumed that this adsorption zone could be related to the deposition of octovalent plutonium in the form of PuO{sub 4}. Later the correctness of this assumption was shown. (orig.)

  7. PLUTONIUM METALLIC FUELS FOR FAST REACTORS

    Energy Technology Data Exchange (ETDEWEB)

    STAN, MARIUS [Los Alamos National Laboratory; HECKER, SIEGFRIED S. [Los Alamos National Laboratory

    2007-02-07

    Early interest in metallic plutonium fuels for fast reactors led to much research on plutonium alloy systems including binary solid solutions with the addition of aluminum, gallium, or zirconium and low-melting eutectic alloys with iron and nickel or cobalt. There was also interest in ternaries of these elements with plutonium and cerium. The solid solution and eutectic alloys have most unusual properties, including negative thermal expansion in some solid-solution alloys and the highest viscosity known for liquid metals in the Pu-Fe system. Although metallic fuels have many potential advantages over ceramic fuels, the early attempts were unsuccessful because these fuels suffered from high swelling rates during burn up and high smearing densities. The liquid metal fuels experienced excessive corrosion. Subsequent work on higher-melting U-PuZr metallic fuels was much more promising. In light of the recent rebirth of interest in fast reactors, we review some of the key properties of the early fuels and discuss the challenges presented by the ternary alloys.

  8. Plutonium and americium monazite materials: Solid state synthesis and X-ray diffraction study

    Energy Technology Data Exchange (ETDEWEB)

    Bregiroux, D. [DEN/DEC/SPUA, Commissariat a l' Energie Atomique, Cadarache, 13108 Saint Paul Lez Durance (France); Laboratoire Science des Procedes Ceramiques et de Traitements de Surface, UMR CNRS-Universite no. 6638, Batiment Chimie, 123 avenue Albert Thomas, 87060 Limoges (France); E-mail: damien.bregiroux@ccr.jussieu.fr; Belin, R. [DEN/DEC/SPUA, Commissariat a l' Energie Atomique, Cadarache, 13108 Saint Paul Lez Durance (France); Valenza, P. [DEN/DEC/SPUA, Commissariat a l' Energie Atomique, Cadarache, 13108 Saint Paul Lez Durance (France); Audubert, F. [DEN/DEC/SPUA, Commissariat a l' Energie Atomique, Cadarache, 13108 Saint Paul Lez Durance (France); Bernache-Assollant, D. [Ecole Nationale Superieure des Mines, 158 Cours Fauriel, 42023 Saint Etienne (France)

    2007-06-30

    High-temperature solid state syntheses of monazite powders containing plutonium (III), plutonium (IV) and americium (III) were performed. Resulting powders were characterized by X-ray diffraction. Pu{sup 3+}PO{sub 4} was readily obtained as a single phase by heating a Pu{sup 4+}O{sub 2}-NH{sub 4}H{sub 2}PO{sub 4} mixture under argon atmosphere. Traces of tetravalent plutonium phosphate Pu{sup 4+}P{sub 2}O{sub 7} were detected when synthesized under air atmosphere. The incorporation of (Pu{sup 4+},Ca{sup 2+}) in the monazite structure was investigated under air and argon atmosphere. We showed that Pu{sup 4+} is fully reduced in Pu{sup 3+} under argon atmosphere whereas, under air, the compound with the formula Pu{sub 0.4}{sup 3+}Pu{sub 0.3}{sup 4+}Ca{sub 0.3}{sup 2+}PO{sub 4} was obtained. Pure Am{sup 3+}PO{sub 4} was also synthesized under argon atmosphere. X-ray patterns revealed a complete amorphisation of the monazite structure at a relatively low cumulative alpha dose for {sup 241}AmPO{sub 4}.

  9. Plutonium and minor actinides recycling in PWRs with new APA concepts

    Energy Technology Data Exchange (ETDEWEB)

    Golfier, H.; Rohart, M.; Aniel, S.; Bergeron, J.; Deffain, J.P. [CEA Saclay, Dept. Modelisation des Systemes et Structures, DM2S, 91 - Gif-sur-Yvette (France)

    2001-07-01

    In the frame of the studies required by the French law of 1991, CEA have launched a wide range of assessments on waste management for different reactors (PWR, FBR). Considerable R and D work has already been performed in order to improve the use of Plutonium (Pu) in PWRs. In this context, the Advanced Plutonium Assembly (APA) aims to improve the use of Plutonium (Pu) in PWRs while minimizing Minor Actinides (MA) production, with only slight modifications of the core design. From a neutronic point of view, the overall studied cases lead to the stabilization of the Pu inventory with approximately 30% of the park refueled with APA assemblies in full APA cores. Multi-recycling could satisfy the stabilization of Pu+ (Am+Cm) inventory by the implementation of approximately 40% APA reactors in a conventional PWRs park. After 7 or 8 recycles, the equilibrium is reached. The Pu inventory in the fuel cycle ranges from 210 tons to 270 tons for Pu multi-recycling, and from 240 tons to 290 tons for Pu+(Am+Cm) multi-recycling. The saving in Natural Uranium and Separative Work Units (SWU) due to the use of APA reactors would be between 30% and 15% in comparison with the UO{sub 2} open cycle. This paper presents a selection of the main preliminary Pu recycling results of the joint study program COGEMA-CEA. (author)

  10. Target fuels for plutonium and minor actinide transmutation in pressurized water reactors

    Energy Technology Data Exchange (ETDEWEB)

    Washington, J., E-mail: jwashing@gmail.com [Nuclear Science and Engineering Program, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401 (United States); King, J., E-mail: kingjc@mines.edu [Nuclear Science and Engineering Program, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401 (United States); Shayer, Z., E-mail: zshayer@mines.edu [Department of Physics, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401 (United States)

    2017-03-15

    Highlights: • We evaluate transmutation fuels for plutonium and minor actinide destruction in LWRs. • We model a modified AP1000 fuel assembly in SCALE6.1. • We evaluate spectral shift absorber coatings to improve transmutation performance. - Abstract: The average nuclear power plant produces twenty metric tons of used nuclear fuel per year, containing approximately 95 wt% uranium, 1 wt% plutonium, and 4 wt% fission products and transuranic elements. Fast reactors are a preferred option for the transmutation of plutonium and minor actinides; however, an optimistic deployment time of at least 20 years indicates a need for a nearer-term solution. This study considers a method for plutonium and minor actinide transmutation in existing light water reactors and evaluates a variety of transmutation fuels to provide a common basis for comparison and to determine if any single target fuel provides superior transmutation properties. A model developed using the NEWT module in the SCALE 6.1 code package provided performance data for the burnup of the target fuel rods in the present study. The target fuels (MOX, PuO{sub 2}, Pu{sub 3}Si{sub 2}, PuN, PuUZrH, PuZrH, PuZrHTh, and PuZrO{sub 2}) are evaluated over a 1400 Effective Full Power Days (EFPD) interval to ensure each assembly remained critical over the entire burnup period. The MOX (5 wt% PuO{sub 2}), Pu{sub 0.31}ZrH{sub 1.6}Th{sub 1.08}, and PuZrO{sub 2}MgO (8 wt% Pu) fuels result in the highest rate of plutonium transmutation with the lowest rate of curium-244 production. This study selected eleven different burnable absorbers (B{sub 4}C, CdO, Dy{sub 2}O{sub 3}, Er{sub 2}O{sub 3}, Eu{sub 2}O{sub 3}, Gd{sub 2}O{sub 3}, HfO{sub 2}, In{sub 2}O{sub 3}, Lu{sub 2}O{sub 3}, Sm{sub 2}O{sub 3}, and TaC) for evaluation as spectral shift absorber coatings on the outside of the fuel pellets to determine if an absorber coating can improve the transmutation properties of the target fuels. The PuZrO{sub 2}MgO (8 wt% Pu) target

  11. Management of disused plutonium sealed sources

    Energy Technology Data Exchange (ETDEWEB)

    Whitworth, Julia Rose [Los Alamos National Laboratory; Pearson, Michael W [Los Alamos National Laboratory; Abeyta, Cristy [Los Alamos National Laboratory

    2010-01-01

    The Global Threat Reduction Initiative's (GTRI) Offsite Source Recovery Project (OSRP) has been recovering excess and unwanted radioactive sealed sources since 1999, including more than 2,400 Plutonium (Pu)-238 sealed sources and 653 Pu-239-bearing sources that represent more than 10% of the total sources recovered by GTRI/OSRP to date. These sources have been recovered from hundreds of sites within the United States (US) and around the world. OSRP grew out of early efforts at the Los Alamos National Laboratory (LANL) to recover and disposition excess Plutonium-239 (Pu-239) sealed sources that were distributed in the 1960s and 1970s under the Atoms for Peace Program, a loan-lease program that serviced 31 countries, as well as domestic users. In the conduct of these recovery operations, GTRI/OSRP has been required to solve problems related to knowledge-of-inventory, packaging and transportation of fissile and heat-source materials, transfer of ownership, storage of special nuclear material (SNM) both at US Department of Energy (DOE) facilities and commercially, and disposal. Unique issues associated with repatriation from foreign countries, including end user agreements required by some European countries and denials of shipment, will also be discussed.

  12. Interstitial incorporation of plutonium into a low-dimensional potassium borate.

    Science.gov (United States)

    Wang, Shuao; Diwu, Juan; Simonetti, Antonio; Booth, Corwin H; Albrecht-Schmitt, Thomas E

    2011-11-01

    The molten boric acid flux reaction of PuBr(3) with KBO(2) at 200 °C results in the formation of large light-yellow crystals of K[B(5)O(7)(OH)(2)]·H(2)O:Pu(4+). Single-crystal X-ray diffraction experiments on the Pu-doped K[B(5)O(7)(OH)(2)]·H(2)O demonstrate two features: (1) K[B(5)O(7)(OH)(2)]·H(2)O:Pu(4+) adopts a one-dimensional borate chain structure with void spaces between the chains. (2) The doping plutonium atoms do not reside on the potassium sites. The latter are not fully occupied. Both laser-ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) and energy-dispersive spectrometry analyses indicate that plutonium atoms are uniformly distributed in crystals of K[B(5)O(7)(OH)(2)]·H(2)O with an atomic K:Pu ratio of approximately 65:1 measured by LA-ICP-MS. UV-vis-NIR spectra taken from both freshly made and one day old crystals show that the plutonium present within the crystals is predominantly characterized by Pu(IV). A small amount of Pu(III) is also present initially, but slowly oxidized to Pu(IV) via interaction with oxygen in the air. X-ray absorption near-edge structure and extended X-ray absorption fine structure spectroscopic measurements confirm that plutonium is mainly present as a form similar to that of a PuO(2) cluster. The combined results suggest that the clusters containing Pu(IV) ions are uniformly distributed in the void spaces between the borate chains.

  13. Exotic new oxides of plutonium found by using gas thermochromatography

    Energy Technology Data Exchange (ETDEWEB)

    Domanov, V.P.; Buklanov, G.V.; Lobanov, Yu.V [Joint Institute for Nuclear Research, Flerov Laboratory of Nuclear Reactions, Dubna, Moscow (Russian Federation)

    2002-11-01

    The volatility of compounds formed during heating of trace quantities of {sup 238}Pu or {sup 239}Pu in a stream of helium and oxygen mixture was studied by gas thermochromatography. Under certain conditions plutonium forms four adsorption zones with the centers at 450{+-}25degC, 250{+-}25degC, 130{+-}50degC and -105{+-}25degC in quartz thermochromatographic(TC) columns. For the interpretation of the results, model experiments with carrier-free radioisotopes of Os, Re, Ru and Tc were performed. It was found that in the stream of He with a small amounts of O{sub 2}, products were adsorbed at 450-500degC and at 250-300degC in the form of dioxides and trioxides. The results of the TC isolation of volatile oxygen-containing compounds of U and {sup 249}Cf are also presented. Based on the data obtained with Pu, we assume that the first adsorption zone (450{+-}25degC) is due to PuO{sub 2} formation, the second one is due to PuO{sub 3} formation and the third may be due to formation of a plutonium acid H{sub 2}PuO{sub 4} (proposed formula). Comparison of the adsorption zone of OsO{sub 4} with the fourth deposition zone for Pu indicates their similarity. We conclude that at -105{+-}25degC, octovalent plutonium deposits in the form of tetraoxide. (author)

  14. LLNL SFA FY11 Program Management and Performance Report: Environmental Transport of Plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Kersting, Annie B. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Powell, Brian A. [Clemson Univ., SC (United States); Moser, Duane [Desert Research Inst. (DRI), Las Vegas, NV (United States); Carroll, Susan A. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Maxwell, Robert [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Dai, Zurong [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Williams, Ross [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Tumey, Scott [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Zhao, Pihong [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Tinnacher, Ruth [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Huang, Patrick [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Kips, Ruth [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Mason, Harris [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Begg, James [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Fisher, Jen [Desert Research Inst. (DRI), Las Vegas, NV (United States); Simpkins, Laura [Clemson Univ., SC (United States); Zimmerman, Trevor [Clemson Univ., SC (United States); Jablonski, Joseph [Clemson Univ., SC (United States); Snow, Matthew [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2011-07-01

    The major challenge in predicting the mobility and transport of plutonium (Pu) is determining the dominant geochemical processes that control its behavior in the subsurface. The reaction chemistry of Pu (i.e., aqueous speciation, solubility, sorptivity, redox chemistry, and affinity for colloidal particles, both abiotic and microbially mediated) is particularly complicated. It is generally thought that due to its low solubility and high sorptivity, Pu migration in the environment occurs only when facilitated by transport on particulate matter (i.e., colloidal particles). Despite the recognized importance of colloid-facilitated transport of Pu, very little is known about the geochemical and biochemical mechanisms controlling Pu-colloid formation and association, particularly at femtomolar Pu concentrations observed at DOE sites. This 5-year program is designed to test the important biogeochemical processes governing colloid-facilitated Pu transport in the field.

  15. Stabilization and immobilization of military plutonium: A non-proliferation perspective

    Energy Technology Data Exchange (ETDEWEB)

    Leventhal, P. [Nuclear Control Institute, Washington, DC (United States)

    1996-05-01

    The Nuclear Control Institute welcomes this DOE-sponsored technical workshop on stabilization and immobilization of weapons plutonium (W Pu) because of the significant contribution it can make toward the ultimate non-proliferation objective of eliminating weapons-usable nuclear material, plutonium and highly enriched uranium (HEU), from world commerce. The risk of theft or diversion of these materials warrants concern, as only a few kilograms in the hands of terrorists or threshold states would give them the capability to build nuclear weapons. Military plutonium disposition questions cannot be addressed in isolation from civilian plutonium issues. The National Academy of Sciences has urged that {open_quotes}further steps should be taken to reduce the proliferation risks posed by all of the world`s plutonium stocks, military and civilian, separated and unseparated...{close_quotes}. This report discusses vitrification and a mixed oxide fuels option, and the effects of disposition choices on civilian plutonium fuel cycles.

  16. U, Pu, and Am nuclear signatures of the Thule hydrogen bomb debris.

    Science.gov (United States)

    Eriksson, Mats; Lindahl, Patric; Roos, Per; Dahlgaard, Henning; Holm, Elis

    2008-07-01

    This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix.

  17. CRITICALITY CURVES FOR PLUTONIUM HYDRAULIC FLUID MIXTURES

    Energy Technology Data Exchange (ETDEWEB)

    WITTEKIND WD

    2007-10-03

    This Calculation Note performs and documents MCNP criticality calculations for plutonium (100% {sup 239}Pu) hydraulic fluid mixtures. Spherical geometry was used for these generalized criticality safety calculations and three geometries of neutron reflection are: {sm_bullet}bare, {sm_bullet}1 inch of hydraulic fluid, or {sm_bullet}12 inches of hydraulic fluid. This document shows the critical volume and critical mass for various concentrations of plutonium in hydraulic fluid. Between 1 and 2 gallons of hydraulic fluid were discovered in the bottom of HA-23S. This HA-23S hydraulic fluid was reported by engineering to be Fyrquel 220. The hydraulic fluid in GLovebox HA-23S is Fyrquel 220 which contains phosphorus. Critical spherical geometry in air is calculated with 0 in., 1 in., or 12 inches hydraulic fluid reflection.

  18. Partitioning and speciation of Pu in the sedimentary rocks aquifer from the deep liquid nuclear waste disposal

    Energy Technology Data Exchange (ETDEWEB)

    Kalmykov, Stepan N. [Lomonosov Moscow State Univ. (Russian Federation). Dept. of Chemistry; Russian Academy of Sciences, Moscow (Russian Federation). Frumkin Institute of Physical Chemistry and Electrochemistry; Russian Academy of Sciences, Moscow (Russian Federation). Vernadsky Institute of Geochemistry and Analytical Chemistry; Vlasova, Irina E.; Romanchuk, Anna Yu.; Presnyakov, Igor A. [Lomonosov Moscow State Univ. (Russian Federation). Dept. of Chemistry; Zakharova, Elena V.; Volkova, Anna G. [Russian Academy of Sciences, Moscow (Russian Federation). Frumkin Institute of Physical Chemistry and Electrochemistry

    2015-06-01

    Plutonium partitioning and speciation was studied under the conditions of a liquid nuclear waste repository site. The dominating effect of corrosion products (Fe and Cr) oxides on plutonium partitioning was established in batch sorption tests at 150 C and by using sequential extraction. Various techniques including Moessbauer spectrometry, XRD and TEM were used to characterize Fe/Cr oxide phases that form both precipitates and surface coatings which sorb plutonium. The sorption and speciation of plutonium was modeled thermodynamically using Pourbaix diagram that takes into account both surface complexation reaction and precipitation of insoluble PuO{sub 2}.

  19. Transport of (137)Cs, (241)Am and Pu isotopes in the Curonian Lagoon and the Baltic Sea.

    Science.gov (United States)

    Lujanienė, G; Remeikaitė-Nikienė, N; Garnaga, G; Jokšas, K; Šilobritienė, B; Stankevičius, A; Šemčuk, S; Kulakauskaitė, I

    2014-01-01

    Activities of (137)Cs, (241)Am and (239,240)Pu were analyzed with special emphasis on better understanding of radionuclide transport from land via the Neman River estuaries to the Baltic Sea and behavior in the marine environment. Although activity concentrations of (137)Cs in water samples collected the Baltic Sea were almost 100 times higher as compared to the Curonian Lagoon, its activities in the bottom sediments were found to be comparable. Activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios indicated a different contribution of the Chernobyl-originated Pu to the suspended particulate matter (SPM) and bottom sediments. The largest amount of the Chernobyl-derived Pu was found in the smallest suspended matter particles of 0.2-1 μm in size collected in the Klaipeda Strait in 2011-2012. The decrease of characteristic activity (238)Pu/(239,240)Pu and atom (240)Pu/(239)Pu ratios towards the global fallout ones in surface soil and the corresponding increase of plutonium (Pu) ratios in the suspended particulate matter and bottom sediments have indicated that the Chernobyl-derived Pu, primarily deposited on the soil surface, was washed out and transported to the Baltic Sea. Behavior of (241)Am was found to be similar to that of Pu isotopes.

  20. Feasibility of Burning Civilian Grade Pu in the Modular HTR with Th Fuel Cycle

    Institute of Scientific and Technical Information of China (English)

    许云林; 经荥清

    2001-01-01

    The Modular High Temperature Gas-Cooled Reactor (HTR) can be usedto burn plutonium fuel to reduce Pu stockpiles because of its inherent safety characteristics and ability to burn a variety of fuel mixtures. The equilibrium core is calculated and analyzed for Pu enriched fuel. Fuel spheres with 7 g heavy metal including the civilian grade Pu and thorium are loaded into the reactor. An enrichment of 11% is chosen to provide the desired equilibrium core reactivity. The fuel and moderator temperature coefficients are both negative. The maximum fuel element temperature during normal operation and during a loss of coolant accident is less than 1500 ℃. 92% of 239Pu will be burnt during nomal operation. Therefore, a thorium fuel cycle in the modular HTR is an effective method for burning civilian grade plutonium.

  1. First-principles elastic constants and phonons of delta-Pu

    DEFF Research Database (Denmark)

    Söderlind, P.; Landa, A.; Sadigh, B.

    2004-01-01

    Elastic constants and zone-boundary phonons of delta-plutonium have been calculated within the density-functional theory. The paramagnetic state of delta-Pu is modeled by disordered magnetism utilizing either the disordered local moment or the special quasirandom structure techniques. The anomalo......Elastic constants and zone-boundary phonons of delta-plutonium have been calculated within the density-functional theory. The paramagnetic state of delta-Pu is modeled by disordered magnetism utilizing either the disordered local moment or the special quasirandom structure techniques....... The anomalously soft C-' as well as a large anisotropy ratio (C-44/C-') of delta-Pu is reproduced by this theoretical model. Also the recently measured phonons for delta-Pu compare relatively well with their theoretical counterpart at the zone boundaries....

  2. Structural characterization of mixed uranium-plutonium co-precipitates and oxides synthesized by oxalic co-conversion route

    Energy Technology Data Exchange (ETDEWEB)

    Arab-Chapelet, B.; De Bruycker, F.; Picart, S.; Leturcq, G.; Grandjean, S. [Laboratoire de Chimie des Actinides, CEA Valrho, bat 399, BP17171, 30207 Bagnols sur Ceze cedex (France)

    2008-07-01

    In this study, mixed uranium(IV)-plutonium(III) oxalate co-precipitates with Pu/(U+Pu) molar ratio equal to 29 and 45% were synthesized and characterized by X-ray powder diffraction (XRD) and Scanning Electron Microscopy (SEM). The thermal conversion step of these co-precipitates into oxide was carried out under argon flow up to 700 deg. C leading to mixed oxides. The structural investigation on these oxides indicates the formation of (U,Pu)O{sub 2} fluorite-type solid solution characterized by a very homogeneous distribution of plutonium and uranium, a controlled oxygen stoichiometry and well-defined morphology of particles. (authors)

  3. Chemical Disposition of Plutonium in Hanford Site Tank Wastes

    Energy Technology Data Exchange (ETDEWEB)

    Delegard, Calvin H. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Jones, Susan A. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2015-05-07

    This report examines the chemical disposition of plutonium (Pu) in Hanford Site tank wastes, by itself and in its observed and potential interactions with the neutron absorbers aluminum (Al), cadmium (Cd), chromium (Cr), iron (Fe), manganese (Mn), nickel (Ni), and sodium (Na). Consideration also is given to the interactions of plutonium with uranium (U). No consideration of the disposition of uranium itself as an element with fissile isotopes is considered except tangentially with respect to its interaction as an absorber for plutonium. The report begins with a brief review of Hanford Site plutonium processes, examining the various means used to recover plutonium from irradiated fuel and from scrap, and also examines the intermediate processing of plutonium to prepare useful chemical forms. The paper provides an overview of Hanford tank defined-waste–type compositions and some calculations of the ratios of plutonium to absorber elements in these waste types and in individual waste analyses. These assessments are based on Hanford tank waste inventory data derived from separately published, expert assessments of tank disposal records, process flowsheets, and chemical/radiochemical analyses. This work also investigates the distribution and expected speciation of plutonium in tank waste solution and solid phases. For the solid phases, both pure plutonium compounds and plutonium interactions with absorber elements are considered. These assessments of plutonium chemistry are based largely on analyses of idealized or simulated tank waste or strongly alkaline systems. The very limited information available on plutonium behavior, disposition, and speciation in genuine tank waste also is discussed. The assessments show that plutonium coprecipitates strongly with chromium, iron, manganese and uranium absorbers. Plutonium’s chemical interactions with aluminum, nickel, and sodium are minimal to non-existent. Credit for neutronic interaction of plutonium with these absorbers

  4. PLUTONIUM METALLOGRAPHY AT LOS ALAMOS

    Energy Technology Data Exchange (ETDEWEB)

    PEREYRA, RAMIRO A. [Los Alamos National Laboratory; LOVATO, DARRYL [Los Alamos National Laboratory

    2007-01-08

    From early days of the Manhattan program to today, scientists and engineers have continued to investigate the metallurgical properties of plutonium (Pu). Although issues like aging was not a concern to the early pioneers, today the reliability of our aging stockpile is of major focus. And as the country moves toward a new generation of weapons similar problems that the early pioneers faced such as compatibility, homogeneity and malleability have come to the forefront. And metallography will continue to be a principle tool for the resolution of old and new issues. Standard metallographic techniques are used for the preparation of plutonium samples. The samples are first cut with a slow speed idamond saw. After mounting in Epon 815 epoxy resin, the samples are ground through 600 grit silicon carbide paper. PF 5070 (a Freon substitute) is used as a coolant, lubricant, and solvent for most operations. Rough mechanical polished is done with 9-{mu} diamond using a nap less cloth, for example nylon or cotton. Final polish is done with 1-{mu} diamond on a nappy cloth such as sylvet. Ethyl alcohol is then used ultrasonically to clean the samples before electro polishing. The sample is then electro-polished and etched in an electrolyte containing 10% nitric acid, and 90% dimethyleneformalmide. Ethyl alcohol is used as a final cleaning agent. Although standard metallographic preparation techniques are used, there are several reasons why metallography of Pu is difficult and challenging. Firstly, because of the health hazards associated with its radioactive properties, sample preparation is conducted in glove boxes. Figure 1 shows the metallography line, in an R and D facility. Since they are designed to be negative in pressure to the laboratory, cross-contamination of abrasives is a major problem. In addition, because of safety concerns and waste issues, there is a limit to the amount of solvent that can be used. Secondly, Pu will readily hydride or oxidize when in contact

  5. Evolving Density and Static Mechanical Properties in Plutonium from Self-Irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Chung, B W; Thompson, S R; Lema, K E; Hiromoto, D S; Ebbinghaus, B B

    2008-07-31

    Plutonium, because of its self-irradiation by alpha decay, ages by means of lattice damage and helium in-growth. These integrated aging effects result in microstructural and physical property changes. Because these effects would normally require decades to measure, studies are underway to assess the effects of extended aging on the physical properties of plutonium alloys by incorporating roughly 7.5 weight % of highly specific activity isotope {sup 238}Pu into the {sup 239}Pu metal to accelerate the aging process. This paper presents updated results of self-irradiation effects on {sup 238}Pu-enriched alloys measured by immersion density, dilatometry, and tensile tests. After nearly 90 equivalent years of aging, both the immersion density and dilatometry show that the enriched alloys continue to decreased in density by {approx}0.002% per year, without void swelling. Quasi-static tensile measurements show that the aging process increases the strength of plutonium alloys.

  6. The role of troublesome components in plutonium vitrification

    Energy Technology Data Exchange (ETDEWEB)

    Li, Hong; Vienna, J.D.; Peeler, D.K.; Hrma, P.; Schweiger, M.J. [Pacific Northwest National Lab., Richland, WA (United States)

    1996-05-01

    One option for immobilizing surplus plutonium is vitrification in a borosilicate glass. Two advantages of the glass form are (1) high tolerance to feed variability and, (2) high solubility of some impurity components. The types of plutonium-containing materials in the United States inventory include: pits, metals, oxides, residues, scrap, compounds, and fuel. Many of them also contain high concentrations of carbon, chloride, fluoride, phosphate, sulfate, and chromium oxide. To vitrify plutonium-containing scrap and residues, it is critical to understand the impact of each component on glass processing and chemical durability of the final product. This paper addresses glass processing issues associated with these troublesome components. It covers solubility limits of chlorine, fluorine, phosphate, sulfate, and chromium oxide in several borosilicate based glasses, and the effect of each component on vitrification (volatility, phase segregation, crystallization, and melt viscosity). Techniques (formulation, pretreatment, removal, and/or dilution) to mitigate the effect of these troublesome components are suggested.

  7. Water Solubility of Plutonium and Uranium Compounds and Residues at TA-55

    Energy Technology Data Exchange (ETDEWEB)

    Reilly, Sean Douglas [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Smith, Paul Herrick [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Jarvinen, Gordon D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Prochnow, David Adrian [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Schulte, Louis D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; DeBurgomaster, Paul Christopher [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Fife, Keith William [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Rubin, Jim [Los Alamos National Lab. (LANL), Los Alamos, NM (United States; Worl, Laura Ann [Los Alamos National Lab. (LANL), Los Alamos, NM (United States

    2016-06-13

    Understanding the water solubility of plutonium and uranium compounds and residues at TA-55 is necessary to provide a technical basis for appropriate criticality safety, safety basis and accountability controls. Individual compound solubility was determined using published solubility data and solution thermodynamic modeling. Residue solubility was estimated using a combination of published technical reports and process knowledge of constituent compounds. The scope of materials considered includes all compounds and residues at TA-55 as of March 2016 that contain Pu-239 or U-235 where any single item in the facility has more than 500 g of nuclear material. This analysis indicates that the following materials are not appreciably soluble in water: plutonium dioxide (IDC=C21), plutonium phosphate (IDC=C66), plutonium tetrafluoride (IDC=C80), plutonium filter residue (IDC=R26), plutonium hydroxide precipitate (IDC=R41), plutonium DOR salt (IDC=R42), plutonium incinerator ash (IDC=R47), uranium carbide (IDC=C13), uranium dioxide (IDC=C21), U3O8 (IDC=C88), and uranium filter residue (IDC=R26). This analysis also indicates that the following materials are soluble in water: plutonium chloride (IDC=C19) and uranium nitrate (IDC=C52). Equilibrium calculations suggest that PuOCl is water soluble under certain conditions, but some plutonium processing reports indicate that it is insoluble when present in electrorefining residues (R65). Plutonium molten salt extraction residues (IDC=R83) contain significant quantities of PuCl3, and are expected to be soluble in water. The solubility of the following plutonium residues is indeterminate due to conflicting reports, insufficient process knowledge or process-dependent composition: calcium salt (IDC=R09), electrorefining salt (IDC=R65), salt (IDC=R71), silica (IDC=R73) and sweepings/screenings (IDC=R78). Solution thermodynamic modeling also indicates that fire suppression water buffered with a

  8. A biogeochemical framework for bioremediation of plutonium(V) in the subsurface environment.

    Science.gov (United States)

    Deo, Randhir P; Rittmann, Bruce E

    2012-07-01

    Accidental release of plutonium (Pu) from storage facilities in the subsurface environment is a concern for the safety of human beings and the environment. Given the complexity of the subsurface environment and multivalent state of Pu, we developed a quantitative biogeochemical framework for bioremediation of Pu(V)O(2) (+) in the subsurface environment. We implemented the framework in the biogeochemical model CCBATCH by expanding its chemical equilibrium for aqueous complexation of Pu and its biological sub-models for including Pu's toxicity and reduction reactions. The quantified framework reveals that most of the Pu(V) is speciated as free Pu(V)O(2) (+) ((aq)), which is a problem if the concentration of free Pu(V)O(2) (+) is ≥28 μM (the half-maximum toxicity value for bacteria able to reduce Pu(V) to Pu(III)PO(4(am))) or ≥250 μM (the full-toxicity value that takes the bioreduction rate to zero). The framework includes bioreduction of Fe(3+) to Fe(2+), which abiotically reduces Pu(V)O(2) (+) to Pu(IV) and then to Pu(III). Biotic (enzymatic) reduction of Pu(V)O(2) (+) directly to Pu(III) by Shewanella alga (S. alga) is also included in the framework. Modeling results also reveal that for formation of Pu(III)PO(4(am)), the desired immobile product, the concentration of coexisting model strong ligand-nitrilotriacetic acid (NTA)-should be less than or equal to the concentration of total Pu(III).

  9. Critical mass studies of plutonium solutions

    Energy Technology Data Exchange (ETDEWEB)

    Kruesi, F.E.; Erkman, J.O.; Lanning, D.D.

    1952-05-19

    The chain reacting conditions for plutonium nitrate in water solution have been examined experimentally for a variety of sizes of spheres and cylinders. The effects on the critical mass of the displacement of hydrogen and the addition of poisons to the fuel were measured in water tamped and bare reactors. In this report the data obtained in the investigation is presented graphically and in tables. Some preliminary analysis has been made yielding the results: (i) the absorption cross-section of Pu{sup 240} is 925 {plus_minus} 200 barns and (ii) the minimum critical mass of Pu{sup 239} in water is 510 grams at concentration of about 33 grams per liter.

  10. Thermophysical properties of coexistent phases of plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Freibert, Franz J [Los Alamos National Laboratory; Mitchell, Jeremy N [Los Alamos National Laboratory; Saleh, Tarik A [Los Alamos National Laboratory; Schwartz, Dan S [Los Alamos National Laboratory

    2009-01-01

    Plutonium is the element with the greatest number of allotropic phases. Thermally induced transformations between these phases are typically characterized by thermal hysteresis and incomplete phase reversion. With Ga substitutal in the lattice, low symmetry phases are replaced by a higher symmetry phase. However, the low temperature Martensitic phase transformation ({delta} {yields} {alpha}{prime}) in Ga stabilized {delta}-phase Pu is characterized by a region of thermal hysteresis which can reach 200 C in extent. These regions of thermal hysteresis offer a unique opportunity to study thermodynamics in inhomogeneous systems of coexistent phases. The results of thermophysical properties measured for samples of inhomogeneous unalloyed and Ga alloyed Pu will be discussed and compared with similar measurements of their single phase constituents.

  11. Thermophysical properties of coexistent phases of plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Freibert, F J; Mitchell, J N; Saleh, T A; Schwartz, D S, E-mail: freibert@lanl.gov, E-mail: jeremy@lanl.gov, E-mail: tsaleh@lanl.gov, E-mail: dschwartz@lanl.gov [Nuclear Materials Science Group, Materials Science and Technology Division, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States)

    2010-03-15

    Plutonium is the element with the greatest number of allotropic phases. Thermally induced transformations between these phases are typically characterized by thermal hysteresis and incomplete phase reversion. With Ga substitutional in the lattice, low symmetry phases are replaced by a higher symmetry phase. However, the low temperature martensitic phase transformation ({delta}{yields}{alpha}') in Ga stabilized {delta}-phase Pu is characterized by a region of thermal hysteresis which can reach 200 deg. C in extent. These regions of thermal hysteresis offer a unique opportunity to study thermodynamics in inhomogeneous systems of coexistent phases. The results of thermophysical properties measured for samples of inhomogeneous unalloyed and Ga alloyed Pu will be discussed and compared with similar measurements of their single phase constituents.

  12. Long-term retrievability and safeguards for immobilized weapons plutonium in geologic storage

    Energy Technology Data Exchange (ETDEWEB)

    Peterson, P.F. [Univ. of California, Berkeley, CA (United States)

    1996-05-01

    If plutonium is not ultimately used as an energy source, the quantity of excess weapons plutonium (w-Pu) that would go into a US repository will be small compared to the quantity of plutonium contained in the commercial spent fuel in the repository, and the US repository(ies) will likely be only one (or two) locations out of many around the world where commercial spent fuel will be stored. Therefore excess weapons plutonium creates a small perturbation to the long-term (over 200,000 yr) global safeguard requirements for spent fuel. There are details in the differences between spent fuel and immobilized w-Pu waste forms (i.e. chemical separation methods, utility for weapons, nuclear testing requirements), but these are sufficiently small to be unlikely to play a significant role in any US political decision to rebuild weapons inventories, or to change the long-term risks of theft by subnational groups.

  13. Potential of thorium-based fuel cycle for PWR core to reduce plutonium and long-term toxicity

    Energy Technology Data Exchange (ETDEWEB)

    Joo, Hyung Kook; Kim, Taek Kyum; Kim, Young Jin [Korea Atomic Energy Research Institute, Taejon (Korea)

    1999-01-01

    The cross section libraries and calculation methods of the participants were inter-compared through the first stage benchmark calculation. The multiplication factor of unit cell benchmark are in good agreement, but there is significant discrepancies of 2.3 to 3.5 %k at BOC and at EOC between the calculated infinite multiplication factors of each participants for the assembly benchmark. Our results with HELIOS show a reasonable agreement with the others except the MTC value at EOC. To verify the potential of the thorium-based fuel to consume the plutonium and to reduce the radioactivity from the spent fuel, the conceptual core with ThO{sub 2}-PuO{sub 2} or MOX fuel were constructed. The composition and quantity of plutonium isotopes and the radioactivity level of spent fuel for conceptual cores were analyzed, and the neutronic characteristics of conceptual cores were also calculated. The nuclear characteristics for ThO{sub 2}-PuO{sub 2} thorium fueled core was similar to MOX fueled core, mainly due to the same seed fuel material, plutonium. For the capability of plutonium consumption, ThO{sub 2}-PuO{sub 2} thorium fuel can consume plutonium 2.1-2.4 times MOX fuel. The fraction of fissile plutonium in the spent ThO{sub 2}-PuO{sub 2} thorium fuel is more favorable in view of plutonium consumption and non-proliferation than MOX fuel. The radioactivity of spent ThO{sub 2}-PuO{sub 2} thorium and MOX fuel batches were calculated. Since plutonium isotopes are dominant for the long-term radioactivity, ThO{sub 2}-PuO{sub 2} thorium has almost the same level of radioactivity as in MOX fuel for a long-term perspective. (author). 22 figs., 11 tabs.

  14. Reactions of plutonium dioxide with water and oxygen-hydrogen mixtures: Mechanisms for corrosion of uranium and plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Haschke, John M.; Allen, Thomas H.; Morales, Luis A.

    1999-06-18

    Investigation of the interactions of plutonium dioxide with water vapor and with an oxygen-hydrogen mixture show that the oxide is both chemically reactive and catalytically active. Correspondence of the chemical behavior with that for oxidation of uranium in moist air suggests that similar catalytic processes participate in the mechanism of moisture-enhanced corrosion of uranium and plutonium. Evaluation of chemical and kinetic data for corrosion of the metals leads to a comprehensive mechanism for corrosion in dry air, water vapor, and moist air. Results are applied in confirming that the corrosion rate of Pu in water vapor decreases sharply between 100 and 200 degrees C.

  15. Properties of plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Ahn, Jin Su; Yoon, Hwan Ki; Min, Kyung Sik; Kim, Hyun Tae; Ahn, Jong Sung; Kwag, Eon Ho; Ryu, Keon Joong [Korea Atomic Energy Research Institute, Daeduk (Korea, Republic of)

    1996-03-01

    Plutonium has unique chemical and physical properties. Its uniqueness in use has led to rare publications, in Korea. This report covers physical aspects of phase change of metal plutonium, mechanical properties, thermal conductivity, etc, chemical aspects of corrosion, oxidation, how to produce plutonium from spent fuels by describing various chemical treatment methods, which are currently used and were used in the past. It also contains characteristics of the purex reprocessing process which is the most widely used nowadays. And show processes to purify and metalize from recovered plutonium solution. Detection and analysis methods are introduced with key pints for handling, critical safety, toxicity, and effects on peoples. This report gives not only a general idea on what plutonium is, rather than deep technical description, but also basic knowledge on plutonium production and safeguards diversion from the view point of nonproliferation. 18 refs. (Author) .new.

  16. DISSOLUTION OF PLUTONIUM METAL USING NITRIC ACID SOLUTIONS CONTAINING POTASSIUM FLUORIDE

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Crowder, M.; Bronikowski, M.

    2007-10-15

    The deinventory and deactivation of the Savannah River Site's (SRS's) FB-Line facility required the disposition of approximately 2000 items from the facility's vaults. Plutonium (Pu) scraps and residues which do not meet criteria for conversion to a mixed oxide fuel will be dissolved and the solution stored for subsequent disposition. Some of the items scheduled for dissolution are composite materials containing Pu and tantalum (Ta) metals. The preferred approach for handling this material is to dissolve the Pu metal, rinse the Ta metal with water to remove residual acid, and burn the Ta metal. The use of a 4 M nitric acid (HNO{sub 3}) solution containing 0.2 M potassium fluoride (KF) was initially recommended for the dissolution of approximately 500 g of Pu metal. However, prior to the use of the flowsheet in the SRS facility, a new processing plan was proposed in which the feed to the dissolver could contain up to 1250 g of Pu metal. To evaluate the use of a larger batch size and subsequent issues associated with the precipitation of plutonium-containing solids from the dissolving solution, scaled experiments were performed using Pu metal and samples of the composite material. In the initial experiment, incomplete dissolution of a Pu metal sample demonstrated that a 1250 g batch size was not feasible in the HB-Line dissolver. Approximately 45% of the Pu was solubilized in 4 h. The remaining Pu metal was converted to plutonium oxide (PuO{sub 2}). Based on this work, the dissolution of 500 g of Pu metal using a 4-6 h cycle time was recommended for the HB-Line facility. Three dissolution experiments were subsequently performed using samples of the Pu/Ta composite material to demonstrate conditions which reduced the risk of precipitating a double fluoride salt containing Pu and K from the dissolving solution. In these experiments, the KF concentration was reduced from 0.2 M to either 0.15 or 0.175 M. With the use of 4 M HNO{sub 3} and a reduction in

  17. Plutonium contamination in soils and sediments at Mayak PA, Russia.

    Science.gov (United States)

    Skipperud, Lindis; Salbu, Brit; Oughton, Deborah H; Drozcho, Eugeny; Mokrov, Yuri; Strand, Per

    2005-09-01

    The Mayak Production Association (Mayak PA) was established in the late 1940's to produce plutonium for the Soviet Nuclear Weapons Programme. In total, seven reactors and two reprocessing plants have been in operation. Today, the area comprises both military and civilian reactors as well as reprocessing and metallurgical plants. Authorized and accidental releases of radioactive waste have caused severe contamination to the surrounding areas. In the present study, [alpha]-spectrometry and inductively coupled plasma-mass spectrometry (ICP-MS) have been used to determine plutonium activities and isotope ratios in soil and sediment samples collected from reservoirs of the Techa River at the Mayak area and downstream Techa River. The objective of the study was to determine the total inventory of plutonium in the reservoirs and to identify the different sources contributing to the plutonium contamination. Results based on [alpha]-spectrometry and ICP-MS measurements show the presence of different sources and confirmed recent reports of civilian reprocessing at Mayak. Determination of activity levels and isotope ratios in soil and sediment samples from the Techa River support the hypothesis that most of the plutonium, like other radionuclides in the Techa River, originated from the very early waste discharges to the Techa River between 1949 and 1951. Analysis of reservoir sediment samples suggest that about 75% of the plutonium isotopes could have been released to Reservoir 10 during the early weapons production operation of the plant, and that the majority of plutonium in Reservoir 10 originates from discharges from power production or reprocessing. Enhanced 240Pu/239Pu atom ratios in river sediment upper layers (0-2 cm) between 50 and 250 km downstream from the plant indicate a contribution from other, non-fallout sources.

  18. PLUTONIUM-ZIRCONIUM ALLOYS

    Science.gov (United States)

    Schonfeld, F.W.; Waber, J.T.

    1960-08-30

    A series of nuclear reactor fuel alloys consisting of from about 5 to about 50 at.% zirconium (or higher zirconium alloys such as Zircaloy), balance plutonium, and having the structural composition of a plutonium are described. Zirconium is a satisfactory diluent because it alloys readily with plutonium and has desirable nuclear properties. Additional advantages are corrosion resistance, excellent fabrication propenties, an isotropie structure, and initial softness.

  19. Pu(V) transport through Savannah River Site soils - an evaluation of a conceptual model of surface- mediated reduction to Pu (IV).

    Science.gov (United States)

    Powell, Brian A; Kaplan, Daniel I; Serkiz, Steven M; Coates, John T; Fjeld, Robert A

    2014-05-01

    Over the last fifteen years the Savannah River Site (SRS) in South Carolina, USA, was selected as the site of three new plutonium facilities: the Mixed Oxide Fuel Fabrication Facility, Pit Disassembly and Conversion Facility, and the Pu Immobilization Plant. In order to assess the potential human and environmental risk associated with these recent initiatives, improved understanding of the fate and transport of Pu in the SRS subsurface environment is necessary. The hypothesis of this study was that the more mobile forms of Pu, Pu(V) and Pu(VI), would be reduced to the less mobile Pu(III/IV) oxidation states under ambient SRS subsurface conditions. Laboratory-scale dynamic flow experiments (i.e., column studies) indicated that Pu(V) was very mobile in SRS sediments. At higher pH values the mobility of Pu decreased and the fraction of Pu that became irreversibly sorbed to the sediment increased, albeit, only slightly. Conversely, these column experiments showed that Pu(IV) was essentially immobile and was largely irreversibly sorbed to the sediment. More than 100 batch sorption experiments were also conducted with four end-member sediments, i.e., sediments that include the chemical, textural, and mineralogical properties likely to exist in the SRS. These tests were conducted as a function of initial Pu oxidation state, pH, and contact time and consistently demonstrated that although Pu(V) sorbed initially quite weakly to sediments, it slowly, over the course of Pu(IV). This is consistent with our hypothesis that Pu(V) is reduced to the more strongly sorbing form of Pu, Pu(IV). These studies provide important experimental support for a conceptual geochemical model for dissolved Pu in a highly weathered subsurface environment. That is that, irrespective of the initial oxidation state of the dissolved Pu introduced into a SRS sediment system, Pu(IV) controls the environmental transport within a couple weeks and Pu strongly binds to the sediment, limiting its mobility.

  20. DETERMINATION OF 237NP AND PU ISOTOPES IN LARGE SOIL SAMPLES BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.

    2010-07-26

    A new method for the determination of {sup 237}Np and Pu isotopes in large soil samples has been developed that provides enhanced uranium removal to facilitate assay by inductively coupled plasma mass spectrometry (ICP-MS). This method allows rapid preconcentration and separation of plutonium and neptunium in large soil samples for the measurement of {sup 237}Np and Pu isotopes by ICP-MS. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via {sup 238}U peak tailing. The method provides enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then transferring Pu to DGA resin for additional purification. The decontamination factor for removal of uranium from plutonium for this method is greater than 1 x 10{sup 6}. Alpha spectrometry can also be applied so that the shorter-lived {sup 238}Pu isotope can be measured successfully. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu and {sup 238}Pu were measured by alpha spectrometry.

  1. Production and characterization of monodisperse plutonium, uranium, and mixed uranium-plutonium particles for nuclear safeguard applications.

    Science.gov (United States)

    Ranebo, Y; Niagolova, N; Erdmann, N; Eriksson, M; Tamborini, G; Betti, M

    2010-05-15

    In order to prevent nuclear proliferation, the isotopic analysis of uranium and plutonium microparticles has strengthened the means in international safeguards for detecting undeclared nuclear activities. In order to ensure accuracy and precision in the analytical methodologies used, the instrumental techniques need to be calibrated. The objective of this study was to produce and characterize particles consisting of U, Pu, and mixed U-Pu, suitable for such reliability verifications. A TSI vibrating orifice aerosol generator in connection with a furnace system was used to produce micrometer sized, monodispersed particles from reference U and Pu materials in solution. The particle masses (in the range of 3-6 pg) and sizes (approximately 1.5 microm) were controlled by the experimental conditions and the parameters for the aerosol generator. Size distributions were obtained from scanning electron microscopy, and energy-dispersive X-ray analysis confirmed that the particle composition agreed with the starting material used. A secondary ion mass spectrometer (SIMS) was used to characterize the isotopic composition of the particles. Isobaric and polyatomic interference in the SIMS spectra was identified. In order to obtain accurate estimates of the interference, a batch of Pu particles were produced of mainly (242)Pu. These were used for SIMS analysis to characterize the relative ionization of Pu and U hydride ions and to determine the SIMS useful yields of U and Pu. It was found that U had a higher propensity to form the hydride than Pu. Useful yields were determined at a mass resolution of 450 for U-Pu particles: (1.71 +/- 0.15) % for Pu and (0.72 +/- 0.06) % for U. For Pu particles: (1.65 +/- 0.14) % for Pu. This gave a relative sensitivity factor between U and Pu (RSF(U:Pu)) of 2.4 +/- 0.2. However, the RSF(U:Pu) showed large fluctuations during the sputtering time for each analyses of the mixed U-Pu particles, in the range of 1.9-3.4.

  2. Disposition of plutonium-239 via production of fission molybdenum-99.

    Science.gov (United States)

    Mushtaq, A

    2011-04-01

    A heritage of physical consequences of the U.S.-Soviet arms race has accumulated, the weapons-grade plutonium (WPu), which will become excess as a result of the dismantlement of the nuclear weapons under the arms reduction agreements. Disposition of Pu has been proposed by mixing WPu with high-level radioactive waste with subsequent vitrification into large, highly radioactive glass logs or fabrication into mixed oxide fuel with subsequent irradiation in existing light water reactors. A potential option may be the production of medical isotope molybdenum-99 by using Pu-239 targets.

  3. Transmission Electron Microscopy Characterization of Helium Bubbles in Aged Plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Schwartz, A J; Wall, M A; Zocco, T G; Blobaum, K M

    2004-11-02

    The self-irradiation damage generated by alpha decay of plutonium results in the formation of lattice defects, helium, and uranium atoms. Over time, microstructural evolution resulting from the self-irradiation may influence the physical and mechanical properties of the material. In order to assess microstructural changes, we have developed and applied procedures for the specimen preparation, handling, and transmission electron microscopy characterization of Pu alloys. These transmission electron microscopy investigations of Pu-Ga alloys ranging in age up to 42-years old reveal the presence of nanometer-sized helium bubbles. The number density of bubbles and the average size have been determined for eight different aged materials.

  4. Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric, E-mail: patriclindahl@yahoo.com [School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL4 8AA (United Kingdom); Worsfold, Paul; Keith-Roach, Miranda [School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL4 8AA (United Kingdom); Andersen, Morten B. [Bristol Isotope Group, School of Earth Sciences, University of Bristol, Wills Memorial Building, Bristol BS8 1RJ (United Kingdom); Kershaw, Peter; Leonard, Kins [The Centre for Environment, Fisheries and Aquaculture Science, Lowestoft Laboratory, Pakefield Road, Suffolk NR33 0HT (United Kingdom); Choi, Min-Seok [Division of Earth and Environmental Science, Korea Basic Science Institute, 113 Gwahangno, Yusung-gu, Daejon 305-333 (Korea, Republic of); Boust, Dominique [Laboratoire de Radioecologie, Institut de Radioprotection et de Surete Nucleaire, BP 10, 50130 Cherbourg-Octeville (France); Lesueur, Patrick [University of Caen Basse Normandie, M2C UMR CNRS 6143, 14000 Caen (France)

    2011-11-01

    A depth profile of {sup 239}Pu and {sup 240}Pu specific activities and isotope ratios was determined in an inter-tidal sediment core from the Esk Estuary in the northeastern Irish Sea. The study site has been impacted with plutonium through routine radionuclide discharges from the Sellafield nuclear reprocessing plant in Cumbria, NW England. A pronounced sub-surface maximum of {approx} 10 kBq kg{sup -1} was observed for {sup 239+240}Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to {approx} 0.04 kBq kg{sup -1} in the deeper layers. The depth profile of {sup 239+240}Pu specific activities together with results from gamma-ray spectrometry for {sup 137}Cs and {sup 241}Am was compared with reported releases from the Sellafield plant in order to estimate a reliable sediment chronology. The upper layers (1992 onwards) showed higher {sup 239+240}Pu specific activities than would be expected from the direct input of annual Sellafield discharges, indicating that the main input of Pu is from the time-integrated contaminated mud patch of the northeastern Irish Sea. The {sup 240}Pu/{sup 239}Pu atom ratios ranged from {approx} 0.03 in the deepest layers to > 0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing {sup 240}Pu/{sup 239}Pu atom ratio with depth reflects the changing nature of operations at the Sellafield plant from weapons-grade Pu production to reprocessing spent nuclear fuel with higher burn-up times in the late 1950s. In addition, recent annual {sup 240}Pu/{sup 239}Pu atom ratios in winkles collected during 2003-2008 from three stations along the Cumbrian coastline showed no significant spatial or temporal differences with an overall average of 0.204, which supports the hypothesis of diluted Pu input from the contaminated mud patch. - Highlights: {yields} Depth profiles of {sup 239}Pu and {sup 240}Pu determined in a northeastern Irish Sea sediment. {yields

  5. Low-Level Plutonium Bioassay Measurements at the Lawrence Livermore National Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Hamilton, T; Brown, T; Hickman, D; Marchetti, A; Williams, R; Kehl, S

    2007-06-18

    Plutonium-239 ({sup 239}Pu) and plutonium-240 ({sup 240}Pu) are important alpha emitting radionuclides contained in radioactive debris from nuclear weapons testing. {sup 239}Pu and {sup 240}Pu are long-lived radionuclides with half-lives of 24,400 years and 6580 years, respectively. Concerns over human exposure to plutonium stem from knowledge about the persistence of plutonium isotopes in the environment and the high relative effectiveness of alpha-radiation to cause potential harm to cells once incorporated into the human body. In vitro bioassay tests have been developed to assess uptakes of plutonium based on measured urinary excretion patterns and modeled metabolic behaviors of the absorbed radionuclides. Systemic plutonium absorbed by the deep lung or from the gastrointestinal tract after ingestion is either excreted or distributed to other organs, primarily to the liver and skeleton, where it is retained for biological half-times of around 20 and 50 years, respectively. Dose assessment and atoll rehabilitation programs in the Marshall Islands have historically given special consideration to residual concentrations of plutonium in the environment even though the predicted dose from inhalation and/or ingestion of plutonium accounts for less than 5% of the annual effective dose from exposure to fallout contamination. Scientists from the Lawrence Livermore National Laboratory (LLNL) have developed a state-of-the-art bioassay test to assess urinary excretion rates of plutonium from Marshallese populations. This new heavy-isotope measurement system is based on Accelerator Mass Spectrometry (AMS). The AMS system at LLNL far exceeds the standard measurement requirements established under the latest United States Department of Energy (DOE) regulation, 10CFR 835, for occupational monitoring of plutonium, and offers several advantages over classical as well as competing new technologies for low-level detection and measurement of plutonium isotopes. The United States

  6. Simplified structure of a new model to describe urinary excretion of plutonium after systemic, liver or pulmonary contamination of rats associated with Ca-DTPA treatments.

    Science.gov (United States)

    Fritsch, P; Sérandour, A L; Grémy, O; Phan, G; Tsapis, N; Abram, M C; Renault, D; Fattal, E; Benech, H; Deverre, J R; Poncy, J L

    2009-06-01

    This study validates, by targeted experiments, several modeling hypotheses for interpretation of urinary excretion of plutonium after Ca-DTPA treatments. Different formulations and doses of Ca-DTPA were administered to rats before or after systemic, liver or lung contamination with various chemical forms of plutonium. The biokinetics of plutonium was also characterized after i.v. injection of Pu-DTPA. Once formed, Pu-DTPA complexes are stable in most biological environments. Pu-DTPA present in circulating fluids is rapidly excreted in the urine, but 2-3% is retained, mainly in soft tissues, and is then excreted slowly in the urine after transfer to blood. Potentially, all intracellular monoatomic forms of plutonium could be decorporated after DTPA internalization involving slow urinary excretion of Pu-DTPA with half-lives varying from 2.5 to 6 days as a function of tissue retention. The ratio of fast to slow urinary excretion of Pu-DTPA depends on both plutonium contamination and Ca-DTPA treatment. Fast urinary excretion of Pu-DTPA corresponds to extracellular decorporation that occurs beyond a threshold of the free DTPA concentration in circulating fluids. Slow excretion corresponds mostly to intracellular decorporation and depends on the amount of intracellular DTPA. From these results, the structure of a simplified model is proposed for interpretation of data obtained with Ca-DTPA treatments after systemic, wound or pulmonary contamination by plutonium.

  7. Development of Pu analysis in high active liquid waste. JASPAS JC-13

    Energy Technology Data Exchange (ETDEWEB)

    Jitsukata, Syu [Joyo Industry Co., Ltd., Tokai, Ibaraki (Japan); Kuno, Takehiko; Sato, Soichi; Ikeda, Hisashi [Japan Nuclear Cycle Development Inst., Tokai, Ibaraki (Japan). Tokai Works; Kurosawa, Akira [Japan Nuclear Fuel Co. Ltd., Tokyo (Japan)

    2001-05-01

    It has been required from IAEA to determine a small amount of plutonium in the high active liquid waste solutions (HALW) in the Tokai reprocessing plant. High performance spectrophotometer (HPSP), which could be obtained lower detection limit than conventional spectrophotometer, is studied to be applied the inspection and verification analysis. The results of applicability test are described in this report. -Cold Test- Neodium, showing an absorption peak near the absorption wavelength of plutonium (VI), was used as an alternative element to plutonium, in order to review the calculation method of the peak intensity. -Hot Test- Plutonium nitrate solution was used for the fundamental test of this method. Since the method is known to be influenced by acidity, suspended sludge and coexistent elements in a sample, each dependency was examined. It was found that measurement results varied about 14% at a nitric acid concentration of 2-4 mol/L. Sludge could be removed by filtration before the measurement. The effect of coexisting elements could be eliminated adjusting the optical balance between reference and sample beam intensity. In the case of measuring a low concentration plutonium solution, a ratio of the peak intensity to the background intensity (S/B ratio) was not enough to the measured low concentration of Plutonium. Therefore a method should be improved the S/B ratio by analyzing the obtained spectra. Data accumulation method, simple moving average method and Fourier transform analysis was tested. The results showed that a combination of the accumulated average method and the moving average method was the optimum method for the purpose. Linearity of the calibration curve was found between 0-11 mgPu/L. Synthetic sample solution, which simulated the actual constituents of the HALW with plutonium, showed a good linear relation at 0-11 mgPu/L. The detection limit for plutonium concentration was 0.07 mgPu/L. When the synthetic HALW solution containing plutonium was

  8. Atomic Structure and Phase Transformations in Pu Alloys

    Energy Technology Data Exchange (ETDEWEB)

    Schwartz, A J; Cynn, H; Blobaum, K M; Wall, M A; Moore, K T; Evans, W J; Farber, D L; Jeffries, J R; Massalski, T B

    2008-04-28

    Plutonium and plutonium-based alloys containing Al or Ga exhibit numerous phases with crystal structures ranging from simple monoclinic to face-centered cubic. Only recently, however, has there been increased convergence in the actinides community on the details of the equilibrium form of the phase diagrams. Practically speaking, while the phase diagrams that represent the stability of the fcc {delta}-phase field at room temperature are generally applicable, it is also recognized that Pu and its alloys are never truly in thermodynamic equilibrium because of self-irradiation effects, primarily from the alpha decay of Pu isotopes. This article covers past and current research on several properties of Pu and Pu-(Al or Ga) alloys and their connections to the crystal structure and the microstructure. We review the consequences of radioactive decay, the recent advances in understanding the electronic structure, the current research on phase transformations and their relations to phase diagrams and phase stability, the nature of the isothermal martensitic {delta} {yields} {alpha}{prime} transformation, and the pressure-induced transformations in the {delta}-phase alloys. New data are also presented on the structures and phase transformations observed in these materials following the application of pressure, including the formation of transition phases.

  9. Plutonium as a tracer for soil erosion assessment in northeast China

    DEFF Research Database (Denmark)

    Xu, Yihong; Qiao, Jixin; Pan, Shaoming;

    2015-01-01

    Soil erosion is one of the most serious environmental and agricultural problems faced by human society. Assessing intensity is an important issue for controlling soil erosion and improving eco-environmental quality. The suitability of the application of plutonium (Pu) as a tracer for soil erosion...... assessment in northeast China was investigated by comparing with that of 137Cs. Here we build on preliminary work, in which we investigated the potential of Pu as a soil erosion tracer by sampling additional reference sites and potential erosive sites, along the Liaodong Bay region in northeast China, for Pu...... in cultivated land. The baseline inventories of 239+240Pu and 137Cs were 88.4 and 1688Bqm-2 respectively. Soil erosion rates estimated by 239+240Pu tracing method were consistent with those obtained by the 137Cs method, confirming that Pu is an effective tracer with a similar tracing behavior to that of 137Cs...

  10. Optimisation of deep burn incineration of reactor waste plutonium in a PBMR DPP-400 core

    Energy Technology Data Exchange (ETDEWEB)

    Serfontein, Dawid E., E-mail: Dawid.Serfontein@nwu.ac.za [School for Mechanical and Nuclear Engineering, North West University, PUK-Campus, Private Bag X6001, Internal Post Box 360, Potchefstroom 2520 (South Africa); Mulder, Eben J. [School for Mechanical and Nuclear Engineering, North West University (South Africa); Reitsma, Frederik [Calvera Consultants (South Africa)

    2014-05-01

    In this article an original set of coupled neutronics and thermo-hydraulic simulation results for the VSOP 99/05 diffusion code are presented for advanced fuel cycles for the incineration of weapons-grade plutonium, reactor-grade plutonium and reactor-grade plutonium with its associated Minor Actinides in the 400 MW{sub th} Pebble Bed Modular Reactor Demonstration Power Plant. These results are also compared to those of the standard 9.6 wt% enriched 9 g/fuel sphere U/Pu fuel cycle. The weapons-grade and reactor-grade plutonium fuel cycles produced good burn-ups. However, the addition of the Minor Actinides to the reactor-grade plutonium caused a large decrease in the burn-up and thus an unacceptable increase in the heavy metal (HM) content in the spent fuel, which was intended for direct disposal in a deep geological repository, without chemical reprocessing. All the plutonium fuel cycles failed the adopted safety limits used in the PBMR400 in that either the maximum fuel temperature of 1130 °C during normal operation, or the maximum power density of 4.5 kW/sphere was exceeded. All the plutonium fuel cycles also produced positive uniform temperature reactivity coefficients, i.e. the reactivity coefficient where the temperatures of the fuel and the graphite moderator in the fuel spheres were varied together. These unacceptable positive coefficients were experienced at low temperatures, typically below 700 °C. This was due to the influence of the thermal fission cross-section resonances of {sup 239}Pu and {sup 241}Pu. Weapons-grade plutonium produced the worst safety performance. The safety performance of the reactor-grade plutonium also deteriorated when the HM loading was reduced from 3 g/sphere to 2 g or 1 g.

  11. Reduction of Pu(VI) on Fe surfaces: soft x-ray absorption and resonant inelastic scattering study

    Energy Technology Data Exchange (ETDEWEB)

    Butorin, S.M.; Kvashnina, K.O.; Modin, A.; Nordgren, J. (Dept. of Physics and Materials Science, Uppsala Univ., Uppsala (Sweden)); Guo, J.H. (Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA (United States)); Shuh, D.K. (Chemical Science Div., Lawrence Berkeley National Laboratory, Berkeley, CA (United States)); Werme, L. (Swedish Nuclear Fuel and Waste Management Co., Stockholm (Sweden))

    2009-03-15

    Based on analysis of spectral shapes, their dependence on the energy of incident photons and comparison with model calculations and experimental data from the reference sample we can conclude that plutonium from the Pu(VI) solution sorbed on Fe surfaces is likely to be reduced and Pu species sorbed on the Fe foils are mainly in the form of Pu (IV). Current results correlate with what was observed for for Np (V) and U (VI) in our previous studies. Furthermore, combined analysis of present data with model atomic multiplet calculations of RIXS and XAS spectra suggests that significant presence of Pu(III) on the Fe foils is unlikely

  12. Compatibility of selected elastomers with plutonium glovebox environment

    Energy Technology Data Exchange (ETDEWEB)

    Burns, R.

    1994-06-01

    This illustrative test was undertaken as a result of on-going failure of elastomer components in plutonium gloveboxes. These failures represent one of the major sources of required maintenance to keep gloveboxes operational. In particular, it was observed that the introduction of high specific activity Pu-238 into a glovebox, otherwise contaminated with Pu-239, resulted in an inordinate failure of elastomer components. Desiring to keep replacement of elastomer components to a minimum, a decision to explore a few possible alternative elastomer candidates was undertaken and reported upon herewith. Sample specimens of Neoprene, Urethane, Viton, and Hypalon elastomeric formulations were obtained from the Bacter Rubber Company. Strips of the elastomer specimens were placed in a plutonium glovebox and outside of a glovebox, and were observed for a period of three years. Of the four types of elastomers, only Hypalon remained completely viable.

  13. Raman spectrum of plutonium dioxide: Vibrational and crystal field modes

    Science.gov (United States)

    Naji, M.; Magnani, N.; Bonales, L. J.; Mastromarino, S.; Colle, J.-Y.; Cobos, J.; Manara, D.

    2017-03-01

    The Raman spectrum of plutonium dioxide is studied both experimentally and theoretically. Particular attention has been devoted to the identification of high-energy modes at 2110 and 2620 c m-1 , whose attribution has so far been controversial. The temperature dependence of both modes suggests an electronic origin for them. Original crystal field (CF) calculations reported in this work show that these two modes can be respectively assigned to the Γ1→Γ5 and Γ1→Γ3 CF transitions within the I54 manifold. These two modes, together with the only vibrational line foreseen by the group theory for the F m -3 m Pu O2 symmetry—the T2 gPu -O stretching mode observed at 478 c m-1 —can thus be used as a Raman fingerprint of fcc plutonium dioxide.

  14. Complexation of Plutonium (IV) With Sulfate At Variable Temperatures

    Energy Technology Data Exchange (ETDEWEB)

    Y. Xia; J.I. Friese; D.A> Moore; P.P. Bachelor; L. Rao

    2006-10-05

    The complexation of plutonium(IV) with sulfate at variable temperatures has been investigated by solvent extraction method. A NaBrO{sub 3} solution was used as holding oxidant to maintain the plutonium(IV) oxidation state throughout the experiments. The distribution ratio of Pu(IV) between the organic and aqueous phases was found to decrease as the concentrations of sulfate were increased. Stability constants of the 1:1 and 1:2 Pu(IV)-HSO{sub 4}{sup -} complexes, dominant in the aqueous phase, were calculated from the effect of [HSO{sub 4}{sup -}] on the distribution ratio. The enthalpy and entropy of complexation were calculated from the stability constants at different temperatures using the Van't Hoff equation.

  15. The relative physiological and toxicological properties of americium and plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Carter, R.E.; Busch, E.; Johnson, O. [and others

    1951-11-15

    The relative physiological and toxicological properties of americium and plutonium have been studied following their intravenous administration to rats. The urinary and fecal excretion of americium was similar to that of plutonium administered as Pu(N0{sub 3}){sub 4}. The deposition of americium the tissues and organs of the rat was also similar to that observed for plutonium. The liver and the skeleton were the major sites of deposition. Zirconium citrate administered 15 minutes after injection of americium increased the urinary excretion of americium and decreased the amount found in the liver and the skeleton at 4 and 16 days. LD{sub 30}{sup 50} studies showed americium was slightly less toxic when given in the acute toxic range than was plutonium. The difference was, however, too slight to be important in establishing a larger tolerance does for americium. Survival studies, hematological observations, bone marrow observations, comparison of tumor incidence and the incidence of skeletal abnormalities indicated that americium and plutonium have essentially the same chronic toxicity when given on an equal {mu}c. basis. These studies support the conclusion that the tolerance values for americium should be essentially the same as those for Plutonium.

  16. Plutonium desorption from mineral surfaces at environmental concentrations of hydrogen peroxide.

    Science.gov (United States)

    Begg, James D; Zavarin, Mavrik; Kersting, Annie B

    2014-06-01

    Knowledge of Pu adsorption and desorption behavior on mineral surfaces is crucial for understanding its environmental mobility. Here we demonstrate that environmental concentrations of H2O2 can affect the stability of Pu adsorbed to goethite, montmorillonite, and quartz across a wide range of pH values. In batch experiments where Pu(IV) was adsorbed to goethite for 21 days at pH 4, 6, and 8, the addition of 5-500 μM H2O2 resulted in significant Pu desorption. At pH 6 and 8 this desorption was transient with readsorption of the Pu to goethite within 30 days. At pH 4, no Pu readsorption was observed. Experiments with both quartz and montmorillonite at 5 μM H2O2 desorbed far less Pu than in the goethite experiments highlighting the contribution of Fe redox couples in controlling Pu desorption at low H2O2 concentrations. Plutonium(IV) adsorbed to quartz and subsequently spiked with 500 μM H2O2 resulted in significant desorption of Pu, demonstrating the complexity of the desorption process. Our results provide the first evidence of H2O2-driven desorption of Pu(IV) from mineral surfaces. We suggest that this reaction pathway coupled with environmental levels of hydrogen peroxide may contribute to Pu mobility in the environment.

  17. New measurement of the 242Pu(n,γ) cross section at n_TOF

    OpenAIRE

    Lerendegui-Marco J.; Guerrero C.; Cortés-Giraldo M. A.; Quesada J.M.; Mendoza E.; Cano-Ott D.; Eberhardt K.; Junghans A.

    2016-01-01

    WONDER-2015 – 4th International Workshop On Nuclear Data Evaluation for Reactor applications The use of MOX fuel (mixed-oxide fuel made of UO2 and PuO2) in nuclear reactors allows substituting a large fraction of the enriched Uranium by Plutonium reprocessed from spent fuel. With the use of such new fuel composition rich in Pu, a better knowledge of the capture and fission cross sections of the Pu isotopes becomes very important. In particular, a new series of cross section evaluations hav...

  18. Reduction of uranium and plutonium oxides by aluminum. Application to the recycling of plutonium; Reduction des oxydes d'uranium et de plutonium par l'aluminium application au recyclage du plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Gallay, J. [Commissariat a l' Energie Atomique, Valduc (France). Centre d' Etudes

    1968-07-01

    A process for treating plutonium oxide calcined at high temperatures (1000 to 2000 deg. C) with a view to recovering the metal consists in the reduction of this oxide dissolved in a mixture of aluminium, sodium and calcium fluorides by aluminium at about 1180 deg. C. The first part of the report presents the results of reduction tests carried out on the uranium oxides UO{sub 2} and U{sub 3}O{sub 8}; these are in agreement with the thermodynamic calculations of the exchange reaction at equilibrium. The second part describes the application of this method to plutonium oxides. The Pu-Al alloy obtained (60 per cent Pu) is then recycled in an aqueous medium. (author) [French] Un procede de traitement de l'oxyde de plutonium calcine a haute temperature (1000 deg. C a 2000 deg. C), en vue de la recuperation du metal, consiste a reduire cet oxyde dissous dans un melange de fluorures d'aluminium, de sodium et de calcium, par l'aluminium vers 1180 deg. C. Une premiere partie du rapport presente les resultats des essais de reduction des oxydes d'uranium UO{sub 2} et U{sub 3}O{sub 8}, en accord avec les resultats du calcul thermodynamique de la reaction d'echange a l'equilibre. Une seconde partie rend compte de l'application de cette methode a l'oxyde de plutonium. L'alliage Pu-Al obtenu (60 pour cent Pu) est ensuite recycle par voie aqueuse. (auteur)

  19. Characteriztion of particulate plutonium released in fuel cycle operations

    Energy Technology Data Exchange (ETDEWEB)

    Seefeldt, W.B.; Mecham, W.J.; Steindler, M.J.

    1976-05-01

    An estimate of the plutonium source terms is made for the fuel cycles of three reactor types on the basis of currently applied, currently available, and estimated future technology. The three reactors are LWR-U, LWR-Pu, and LMFBR. The source terms are characterized as to quantity, form, and particle size distribution. Historical operating data for existing plants and the state of the art of the technology of air cleaning are reviewed.

  20. An improvement in APOR process I-uranium/plutonium separation process

    Institute of Scientific and Technical Information of China (English)

    肖松涛; 李丽; 叶国安; 罗方祥; 刘协春; 杨贺; 兰天

    2015-01-01

    The reduction stripping behavior of Pu(IV) from 30%TBP/OK with hydroxysemicarbazide (HSC) was inves-tigated, and the separation efficiency of HSC and DMHAN-MMH for U/Pu partitioning in Purex process was compared. The results show that HSC can effectively realize the separation of Pu from U;using mixer-settlers to simulate U/Pu separation in 1B bank of PUREX, from 16-stage counter current extraction experiment (in which 6 stages for supplemental extraction, 10 stages for stripping) with flow rate ratio (1BF:1BX:1BS)=4:1:1 in 1B contactor, good result was achieved that the yields are both more than 99.99%for uranium and Pu, the separation factor of plutonium from uranium (SFPu/U) is 2.8 × 104, and separation factor of uranium from plu-tonium (SFU/Pu) is 5.9 × 104. As a stripping reductant, HSC can effectively achieve the separation of Pu from U and the separation effect is nearly the same with DMHAN-MMH, which contributed to replace enough the latter with HSC in the U/Pu separation in Advanced Purex Process Based on Organic Reagent (APOR) process.

  1. Looking Through the Trade Surplus Prism

    Institute of Scientific and Technical Information of China (English)

    2008-01-01

    @@ Huge trade surplus attracks more and more attention to the China's economy operation,a controversial topic on people's lips as well. The years from 2005 to 2007,China's most rapid trade surplus growing period,have witnessed China's continuous trade surplus growing,breaking out the threshold of US$100 billion,and 200 billion US Dollar successivcly.

  2. Behind the Ever-Widening Trade Surplus

    Institute of Scientific and Technical Information of China (English)

    Guo Yan

    2007-01-01

    @@ China's trade surplus has been on the rise since 2005.The surplus hit US$ 32.1 billion in 2004,and has soared to us$177.5 billion in 2006.The Chinese government has made the reduction of the trade surplus one of its major macro-economic goals since last September.

  3. PLUTONIUM-CERIUM-COBALT AND PLUTONIUM-CERIUM-NICKEL ALLOYS

    Science.gov (United States)

    Coffinberry, A.S.

    1959-08-25

    >New plutonium-base teroary alloys useful as liquid reactor fuels are described. The alloys consist of 10 to 20 atomic percent cobalt with the remainder plutonium and cerium in any desired proportion, with the plutonium not in excess of 88 atomic percent; or, of from 10 to 25 atomic percent nickel (or mixture of nickel and cobalt) with the remainder plutonium and cerium in any desired proportion, with the plutonium not in excess of 86 atomic percent. The stated advantages of these alloys over unalloyed plutonium for reactor fuel use are a lower melting point and a wide range of permissible plutonium dilution.

  4. Plutonium storage criteria

    Energy Technology Data Exchange (ETDEWEB)

    Chung, D. [Scientech, Inc., Germantown, MD (United States); Ascanio, X. [Dept. of Energy, Germantown, MD (United States)

    1996-05-01

    The Department of Energy has issued a technical standard for long-term (>50 years) storage and will soon issue a criteria document for interim (<20 years) storage of plutonium materials. The long-term technical standard, {open_quotes}Criteria for Safe Storage of Plutonium Metals and Oxides,{close_quotes} addresses the requirements for storing metals and oxides with greater than 50 wt % plutonium. It calls for a standardized package that meets both off-site transportation requirements, as well as remote handling requirements from future storage facilities. The interim criteria document, {open_quotes}Criteria for Interim Safe Storage of Plutonium-Bearing Solid Materials{close_quotes}, addresses requirements for storing materials with less than 50 wt% plutonium. The interim criteria document assumes the materials will be stored on existing sites, and existing facilities and equipment will be used for repackaging to improve the margin of safety.

  5. Determination of {sup 238}Pu, {sup 239+240}Pu, {sup 241}Pu and {sup 241}Am in radioactive waste from IPEN reactor

    Energy Technology Data Exchange (ETDEWEB)

    Geraldo, Bianca; Taddei, Maria Helena T.; Cheberle, Sandra M.; Ferreira, Marcelo T., E-mail: bgeraldo@cnen.gov.b, E-mail: mhtaddei@cnen.gov.b, E-mail: scsantos@cnen.gov.b, E-mail: ferreira@cnen.gov.b [Brazilian Nuclear Energy Commission (LAPOC/CNEN-MG), Pocos de Caldas, MG (Brazil). Lab. of Pocos de Caldas; Marumo, Julio T., E-mail: jtmarumo@ipen.b [Instituto de Pesquisas Energeticas e Nucleares (IPEN/CNEN-SP), Sao Paulo, SP (Brazil)

    2011-07-01

    Ion exchange resin is a common type of radioactive waste arising from treatment of coolant water of the main circuit of research and nuclear power reactors. This waste contains high concentrations of fission and activation products. The management of this waste includes its characterization in order to determine and quantify specific radionuclides including those known as difficult-to-measure radionuclides (RDM). The analysis of RDMs generally involves expensive and time-consuming complex radiochemical analysis for purification and separation of the radionuclides. The objective of this work is to show an easy methodology for quantifying plutonium and americium isotopes in spent ion exchange resin, used for purification of the cooling water of the IEA-R1 reactor located at the Nuclear and Energy Research Institute, IPEN-CNEN/SP. The resins were destroyed by acid digestion, followed by purification and separation of the Pu and Am isotopes with anionic and chromatographic resins. {sup 238}Pu, {sup 239}+{sup 24}'0Pu, and {sup 24}'1Am isotopes were analyzed in an alpha spectrometer equipped with surface barrier detectors. {sup 241}Pu isotope was analyzed by liquid scintillation counting. Chemical recovery yield ranged from 73 to 98% for Pu and 77 to 98% for Am, demonstrating that the methodology is suitable for identification and quantification of the isotopes studied in spent resins. (author)

  6. Pre-separation of U, Np, Pu in 1AW Samplefor XRF Analysis

    Institute of Scientific and Technical Information of China (English)

    DENG; Wei-qin; TAN; Shu-ping; TAO; Miao-miao; WU; Ji-zong

    2013-01-01

    1AW is the liquid waste of the first separation unit of Purex process.The analysis of U,Np,Pu in1AW contributes to some key points,such as,the recovery of plutonium and uranium,the distribution of neptunium,the control of process.Due to the high radioactivity of 1AW,which accumulated the most

  7. LAB-SCALE DEMONSTRATION OF PLUTONIUM PURIFICATION BY ANION EXCHANGE, PLUTONIUM (IV) OXALATE PRECIPITATION, AND CALCINATION TO PLUTONIUM OXIDE TO SUPPORT THE MOX FEED MISSION

    Energy Technology Data Exchange (ETDEWEB)

    Crowder, M.; Pierce, R.

    2012-08-22

    H-Canyon and HB-Line are tasked with the production of PuO{sub 2} from a feed of plutonium metal. The PuO{sub 2} will provide feed material for the MOX Fuel Fabrication Facility. After dissolution of the Pu metal in H-Canyon, the solution will be transferred to HB-Line for purification by anion exchange. Subsequent unit operations include Pu(IV) oxalate precipitation, filtration and calcination to form PuO{sub 2}. This report details the results from SRNL anion exchange, precipitation, filtration, calcination, and characterization tests, as requested by HB-Line1 and described in the task plan. This study involved an 80-g batch of Pu and employed test conditions prototypical of HB-Line conditions, wherever feasible. In addition, this study integrated lessons learned from earlier anion exchange and precipitation and calcination studies. H-Area Engineering selected direct strike Pu(IV) oxalate precipitation to produce a more dense PuO{sub 2} product than expected from Pu(III) oxalate precipitation. One benefit of the Pu(IV) approach is that it eliminates the need for reduction by ascorbic acid. The proposed HB-Line precipitation process involves a digestion time of 5 minutes after the time (44 min) required for oxalic acid addition. These were the conditions during HB-line production of neptunium oxide (NpO{sub 2}). In addition, a series of small Pu(IV) oxalate precipitation tests with different digestion times were conducted to better understand the effect of digestion time on particle size, filtration efficiency and other factors. To test the recommended process conditions, researchers performed two nearly-identical larger-scale precipitation and calcination tests. The calcined batches of PuO{sub 2} were characterized for density, specific surface area (SSA), particle size, moisture content, and impurities. Because the 3013 Standard requires that the calcination (or stabilization) process eliminate organics, characterization of PuO{sub 2} batches monitored the

  8. Plutonium in a grassland ecosystem. [Rocky Flats Plant

    Energy Technology Data Exchange (ETDEWEB)

    Little, C.A.

    1976-08-01

    A study was made of plutonium contamination of grassland at the Rocky Flats plant northwest of Denver, Colorado. Of interest were: the definition of major plutonium-containing ecosystem compartments; the relative amounts in those compartments; how those values related to studies done in other geographical areas; whether or not the predominant isotopes, /sup 238/Pu and /sup 239/Pu, behaved differently; and what mechanisms might have allowed for the observed patterns of contamination. Samples of soil, litter, vegetation, arthropods, and small mammals were collected for Pu analysis and mass determination from each of two macroplots. Small aliquots (5 g or less) were analyzed by a rapid liquid scintillation technique and by alpha spectrometry. Of the compartments sampled, greater than 99 percent of the total plutonium was contained in the soil and the concentrations were significantly inversely correlated with distance from the contamination source, depth of the sample, and particle size of the sieved soil samples. The soil data suggested that the distribution of contamination largely resulted from physical transport processes.

  9. Simultaneous measurements of plutonium and uranium in spent-fuel dissolver solutions

    Energy Technology Data Exchange (ETDEWEB)

    Li, T.K. [Los Alamos National Lab., NM (United States); Kuno, T.; Kitagawa, O.; Sato, S.; Kurosawa, A.; Kuno, Y. [Power Reactor and Nuclear Fuel Development Corp., Tokai, Ibaraki (Japan)

    1997-11-01

    The authors have studied the isotope dilution gamma-ray spectrometry (IDGS) technique for simultaneous measurements of elemental concentrations and isotopic compositions for both plutonium and uranium in input spent-fuel dissolver solutions at a reprocessing plant. The technique under development includes both sample preparation and analysis methods. For simultaneous measurements of both plutonium and uranium, a critical issue is to develop a new method to keep both plutonium and uranium in the sample after they are separated from fission products. Furthermore, it is equally important to improve the analysis method so that the precision and accuracy of the plutonium analysis remain unaffected while uranium is retained in the sample. To keep both plutonium and uranium in the sample for simultaneous measurements, extraction chromatography is being studied and shows promise to achieve the goal of cosegregation of the plutonium and uranium. The technique uses U/TEVA{center_dot}Spec resin to separate fission products and recover both uranium and plutonium in the resin from dissolver solutions for subsequent measuring using high-resolution gamma-ray spectrometry. Owing to the fact that the U/Pu ratio is altered during the fission product separation phase, it is necessary to develop a method which could accurately correct for this effect. Such a method was developed using the unique decay properties of {sup 241}Pu to {sup 237}U and shows considerable promise in allowing for accurate determination of the {sup 235}U concentrations before the chemical extraction.

  10. Isotope ratio analysis of individual sub-micrometer plutonium particles with inductively coupled plasma mass spectrometry.

    Science.gov (United States)

    Esaka, Fumitaka; Magara, Masaaki; Suzuki, Daisuke; Miyamoto, Yutaka; Lee, Chi-Gyu; Kimura, Takaumi

    2010-12-15

    Information on plutonium isotope ratios in individual particles is of great importance for nuclear safeguards, nuclear forensics and so on. Although secondary ion mass spectrometry (SIMS) is successfully utilized for the analysis of individual uranium particles, the isobaric interference of americium-241 to plutonium-241 makes difficult to obtain accurate isotope ratios in individual plutonium particles. In the present work, an analytical technique by a combination of chemical separation and inductively coupled plasma mass spectrometry (ICP-MS) is developed and applied to isotope ratio analysis of individual sub-micrometer plutonium particles. The ICP-MS results for individual plutonium particles prepared from a standard reference material (NBL SRM-947) indicate that the use of a desolvation system for sample introduction improves the precision of isotope ratios. In addition, the accuracy of the (241)Pu/(239)Pu isotope ratio is much improved, owing to the chemical separation of plutonium and americium. In conclusion, the performance of the proposed ICP-MS technique is sufficient for the analysis of individual plutonium particles.

  11. Survey of plutonium and uranium atom ratios and activity levels in Mortandad Canyon

    Energy Technology Data Exchange (ETDEWEB)

    Gallaher, B.M.; Benjamin, T.M.; Rokop, D.J.; Stoker, A.K.

    1997-09-22

    For more than three decades Mortandad Canyon has been the primary release area of treated liquid radioactive waste from the Los Alamos National Laboratory (Laboratory). In this survey, six water samples and seven stream sediment samples collected in Mortandad Canyon were analyzed by thermal ionization mass spectrometry (TIMS) to determine the plutonium and uranium activity levels and atom ratios. Be measuring the {sup 240}Pu/{sup 239}Pu atom ratios, the Laboratory plutonium component was evaluated relative to that from global fallout. Measurements of the relative abundance of {sup 235}U and {sup 236}U were also used to identify non-natural components. The survey results indicate the Laboratory plutonium and uranium concentrations in waters and sediments decrease relatively rapidly with distance downstream from the major industrial sources. Plutonium concentrations in shallow alluvial groundwater decrease by approximately 1000 fold along a 3000 ft distance. At the Laboratory downstream boundary, total plutonium and uranium concentrations were generally within regional background ranges previously reported. Laboratory derived plutonium is readily distinguished from global fallout in on-site waters and sediments. The isotopic ratio data indicates off-site migration of trace levels of Laboratory plutonium in stream sediments to distances approximately two miles downstream of the Laboratory boundary.

  12. Investigation of plutonium concentration and distribution in burrowing crayfish from the White Oak Creek floodplain

    Energy Technology Data Exchange (ETDEWEB)

    Delaney, M.S.; Dahlman, R.C.; Craig, R.B.

    1979-01-01

    The White Oak floodplain was contaminated with several radionuclides, including /sup 239/Pu, during the Manhattan Project in 1944. Plutonium distribution in the soil is nonhomogeneous. An investigation was conducted to deterine Pu accumulation in a resident animal population. Crayfish were chosen because they complete their life-cycle within the contaminated environment, they directly contact contaminated muds, and they function in a food chain of significance to man. Two major conclusions of the research were that Pu concentrations in contaminated crayfish typically exceed those of control crayfish by two orders of magnitude and that if an incident were to occur in which a standard man ingested the soft tissues of ten crayfish from the floodplain, an insignificant whole body dose would accrue over the subsequent 50 years of life. The digestive tract of contaminated crayfish contained 21 to 33% of the Pu body burden, soft tissues contained 11 to 31% of the Pu body burden, and 48 to 62% of the Pu body burden of contaminated crayfish was associated with the carapace. Therefore, at a molt a large proportion of its accumulated Pu is deposited in the environment. A supplementary laboratory investigation using /sup 237/Pu included a chronic Pu uptake study by uncontaminated crayfish. In these crayfish, from 64 to 82% of the /sup 237/Pu was associated with the body tissues. Complementary data for /sup 237/Pu associated with the carapace ranged from 18 to 37% of the distribution. An inventory of /sup 239/Pu in crayfish at two sites on the floodplain was calculated by multiplying the estimated biomass of the crayfish by their average /sup 239/Pu concentration. This evaluation of Pu associated with the crayfish population was compared to an inventory of /sup 239/Pu in the soil in which they burrow and was found to be eight orders of magnitude less.

  13. Rapid and simultaneous determination of neptunium and plutonium isotopes in environmental samples by extraction chromatography using sequential injection analysis and ICP-MS

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per

    2010-01-01

    This paper reports an automated analytical method for rapid and simultaneous determination of plutonium isotopes (239Pu and 240Pu) and neptunium (237Np) in environmental samples. An extraction chromatographic column packed with TrisKem TEVA® resin was incorporated in a sequential injection (SI...

  14. A Plutonium-Contaminated Wound, 1985, USA

    Energy Technology Data Exchange (ETDEWEB)

    Doran M. Christensen, DO, REAC/TS Associate Director and Staff Physician Eugene H. Carbaugh, CHP, Staff Scientist, Internal Dosimetry Manager, Pacific Northwest National Laboratory, Richland, Washington

    2012-02-02

    A hand injury occurred at a U.S. facility in 1985 involving a pointed shaft (similar to a meat thermometer) that a worker was using to remove scrap solid plutonium from a plastic bottle. The worker punctured his right index finger on the palm side at the metacarpal-phalangeal joint. The wound was not through-and- through, although it was deep. The puncture wound resulted in deposition of ~48 kBq of alpha activity from the weapons-grade plutonium mixture with a nominal 12 to 1 Pu-alpha to {sup 241}Am-alpha ratio. This case clearly showed that DTPA was very effective for decorporation of plutonium and americium. The case is a model for management of wounds contaminated with transuranics: (1) a team approach for dealing with all of the issues surrounding the incident, including the psychological, (2) early surgical intervention for foreign-body removal, (3) wound irrigation with DTPA solution, and (4) early and prolonged DTPA administration based upon bioassay and in vivo dosimetry.

  15. Guide to good practices at plutonium facilities

    Energy Technology Data Exchange (ETDEWEB)

    Faust, L.G.; Brackenbush, L.W.; Carter, L.A.; Endres, G.W.R.; Glenn, R.D.; Jech, J.J.; Selby, J.M.; Smith, R.C.; Waite, D.A.; Walsh, W.P.

    1977-09-01

    This manual establishes guidelines and principles for use in setting up a sound radiation protection program for work with plutonium. The guidance presented is based on the experiences of Energy Research and Development Administration (ERDA) contractors and those portions of private industry concerned with the operation of plutonium facilities, specifically with the fabrication of mixed oxide reactor fuel. The manual is directed primarily to those facilities which have as their sole purpose the handling of large quantities of plutonium for military or industrial uses. It is not intended for use by facilities engaged in reactor or chemical separation operations nor for partial or occasional use by analytical laboratories; while these facilities would find the manual beneficial, it would be incomplete for their needs. The manual addresses good practices that should be observed by management, staff and designers, since the benefits of a good radiation protection program are the result of their joint efforts. Methods for the diagnostic evaluation of internally deposited Pu are included.

  16. Sequential injection approach for simultaneous determination of ultratrace plutonium and neptunium in urine with accelerator mass spectrometry

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per;

    2013-01-01

    An analytical method was developed for simultaneous determination of ultratrace level plutonium (Pu) and neptunium (Np) using iron hydroxide coprecipitation in combination with automated sequential injection extraction chromatography separation and accelerator mass spectrometry (AMS) measurement...... show that preboiling and aging are important for obtaining high chemical yields for both Pu and Np, which is possibly related to the aggregation and adsorption behavior of organic substances contained in urine. Although the optimal condition for Np and Pu simultaneous determination requires 5-day aging...... time, an immediate coprecipitation without preboiling and aging could also provide fairly satisfactory chemical yields for both Np and Pu (50-60%) with high sample throughput (4 h/sample). Within the developed method, (242)Pu was exploited as chemical yield tracer for both Pu and Np isotopes. (242)Pu...

  17. Biokinetics of plutonium-238 injected in non-human primates

    Science.gov (United States)

    Chelidze, Nino

    Seventeen intravenously injected monkey data were analyzed using PowerBasic and SAAM II softwares. The study was divided into three parts. In the first part SAAM II predictions were compared with those calculated by Birchall algorithm based on the ICRP 67 systemic model for plutonium. In the second part SAAM II simulations were performed and compared for two representations of systemic model for plutonium: the ICRP 67 model and the Leggett model. In the third part, optimization of transfer rates suggested by ICRP 67 and Leggett models were attempted by solving each monkey case independently. The Birchall algorithm and SAAM II predicted values coincide with each other for all data presented: blood, urine and feces. Unfortunately, these predictions do not coincide with the measurement values. Plutonium activity in liver is about 50% of the injected activity. The uptake of plutonium in liver in primates seems to be close to the assumption of equal distribution of 45% plutonium in liver and skeleton in humans. For longer sacrificed monkeys we have prolonged liver retention compared to plutonium liver retention in humans. Pu retention in urine and blood has been simulated based on the ICRP 67 and Leggett models respectively and plotted against the measured data points to acquire the understanding of the models with respect to reality. Pu activity was also evaluated in liver and skeleton at the time of the sacrifice for both models and compared with the autopsy measurements for individual cases. Optimization of transfer rates suggested in the ICRP 67 and Leggett models was attempted. Default transfer rates were varied to improve the fits to the data and predict activities in the liver and skeleton at the time of death has been carried out in SAAM II. Good fits for the individual cases were obtained successfully, however, consistency among parameters from case to case was not observed.

  18. Pertubation in the 240Pu/239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain)

    DEFF Research Database (Denmark)

    Mitchell, P.I.; León Vintró, L.; Dahlgaard, H.

    1997-01-01

    been subjected to close-in fallout, mainly from surface-based testing (e.g. Bikini Atoll, Nevada test site, Mururoa Atoll), has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the Pu-240/Pu-239 ratio has been examined...

  19. Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site

    Energy Technology Data Exchange (ETDEWEB)

    Buck, Edgar C.; Moore, Dean A.; Czerwinski, Kenneth R.; Conradson, Steven D.; Batuk, Olga; Felmy, Andrew R.

    2014-08-06

    The occurrence of plutonium dioxide (PuO2) either from direct deposition or from the precipitation of plutonium-bearing solutions in contaminated soils and sediments has been well described, particularly for the Hanford site in Washington State. However, past research has suggested that plutonium may exist in environmental samples at the Hanford site in chemical forms in addition to large size PuO2 particles and that these previously unidentified nano-sized particles maybe more reactive and thus more likely to influence the environmental mobility of Pu. Here we present evidence for the formation of nano-sized plutonium iron phosphate hydroxide structurally related to the rhabdophane group nanoparticles in 216-Z9 crib sediments from Hanford using transmission electron microscopy (TEM). The distribution and nature of these nanoparticles varied depending on the adjacent phases present. Fine electron probes were used to obtain electron diffraction and electron energy-loss spectra from specific phase regions of the 216-Z9 cribs specimens from fine-grained plutonium oxide and phosphate phases. Energy-loss spectra were used to evaluate the plutonium N4,5 (4d → 5f ) and iron L2,3 absorption edges. The iron plutonium phosphate formation may depend on the local micro-environment in the sediments, availability of phosphate, and hence the distribution of these minerals may control long-term migration of Pu in the soil. This study also points to the utility of using electron beam methods for determining the identity of actinide phases and their association with other sediment phases.

  20. Weapons plutonium for electricity: a win-win-win solution

    Energy Technology Data Exchange (ETDEWEB)

    Goldschmidt, P. [Synatom, Brussels (Belgium)

    1997-12-31

    Incorporating recovered weapons-grade plutonium into mixed-oxide (MOX) fuel to produce electricity in currently operating reactors is presented as the best option for its disposition from a European utilities perspective. It would be a win-win-win solution. Firstly, it would be a win for the US government as the only technology readily available on an industrial scale and therefore the fastest way to convert the surplus plutonium to a highly proliferation resistant spent fuel form, as well as being the most cost-effective option. It would also have the political advantages of proving to the world that the US is dedicated to the elimination of its surplus plutonium without delay, receiving support from the Western allies of the US, and encouraging the Russians to take the same route. Secondly, it would be a win for the US utilities both in economic terms and in improving their public image through their contribution to world disarmament. Finally, it would be a win for the world as the fastest route to making disarmament irreversible and as the only solution that conserves natural resources. (8 figures; 14 references) (UK).

  1. Oxygen diffusion model of the mixed (U,Pu)O2 ± x: Assessment and application

    Science.gov (United States)

    Moore, Emily; Guéneau, Christine; Crocombette, Jean-Paul

    2017-03-01

    The uranium-plutonium (U,Pu)O2 ± x mixed oxide (MOX) is used as a nuclear fuel in some light water reactors and considered for future reactor generations. To gain insight into fuel restructuring, which occurs during the fuel lifetime as well as possible accident scenarios understanding of the thermodynamic and kinetic behavior is crucial. A comprehensive evaluation of thermo-kinetic properties is incorporated in a computational CALPHAD type model. The present DICTRA based model describes oxygen diffusion across the whole range of plutonium, uranium and oxygen compositions and temperatures by incorporating vacancy and interstitial migration pathways for oxygen. The self and chemical diffusion coefficients are assessed for the binary UO2 ± x and PuO2 - x systems and the description is extended to the ternary mixed oxide (U,Pu)O2 ± x by extrapolation. A simulation to validate the applicability of this model is considered.

  2. Critical experiments on single-unit spherical plutonium geometries reflected and moderated by oil

    Energy Technology Data Exchange (ETDEWEB)

    Rothe, R.E.

    1997-05-01

    Experimental critical configurations are reported for several dozen spherical and hemispherical single-unit assemblies of plutonium metal. Most were solid but many were hollow-centered, thick, shell-like geometries. All were constructed of nested plutonium (mostly {sup 2139}Pu) metal hemispherical shells. Three kinds of critical configurations are reported. Two required interpolation and/or extrapolation of data to obtain the critical mass because reflector conditions were essentially infinite. The first finds the plutonium essentially fully reflected by a hydrogen-rich oil; the second is essentially unreflected. The third kind reports the critical oil reflector height above a large plutonium metal assembly of accurately known mass (no interpolation required) when that mass was too great to permit full oil reflection. Some configurations had thicknesses of mild steel just outside the plutonium metal, separating it from the oil. These experiments were performed at the Rocky Flats Critical Mass Laboratory in the late 1960s. They have not been published in a form suitable for benchmark-quality comparisons against state-of-the-art computational techniques until this paper. The age of the data and other factors lead to some difficulty in reconstructing aspects of the program and may, in turn, decrease confidence in certain details. Whenever this is true, the point is acknowledged. The plutonium metal was alpha-phase {sup 239}Pu containing 5.9 wt-% {sup 240}Pu. All assemblies were formed by nesting 1.667-mm-thick (nominal) bare plutonium metal hemispherical shells, also called hemishells, until the desired configuration was achieved. Very small tolerance gaps machined into radial dimensions reduced the effective density a small amount in all cases. Steel components were also nested hemispherical shells; but these were nominally 3.333-mm thick. Oil was used as the reflector because of its chemical compatibility with plutonium metal.

  3. Plutonium radiation surrogate

    Science.gov (United States)

    Frank, Michael I [Dublin, CA

    2010-02-02

    A self-contained source of gamma-ray and neutron radiation suitable for use as a radiation surrogate for weapons-grade plutonium is described. The source generates a radiation spectrum similar to that of weapons-grade plutonium at 5% energy resolution between 59 and 2614 keV, but contains no special nuclear material and emits little .alpha.-particle radiation. The weapons-grade plutonium radiation surrogate also emits neutrons having fluxes commensurate with the gamma-radiation intensities employed.

  4. Plutonium Vulnerability Management Plan

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1995-03-01

    This Plutonium Vulnerability Management Plan describes the Department of Energy`s response to the vulnerabilities identified in the Plutonium Working Group Report which are a result of the cessation of nuclear weapons production. The responses contained in this document are only part of an overall, coordinated approach designed to enable the Department to accelerate conversion of all nuclear materials, including plutonium, to forms suitable for safe, interim storage. The overall actions being taken are discussed in detail in the Department`s Implementation Plan in response to the Defense Nuclear Facilities Safety Board (DNFSB) Recommendation 94-1. This is included as Attachment B.

  5. PLUTONIUM SEPARATION METHOD

    Science.gov (United States)

    Beaufait, L.J. Jr.; Stevenson, F.R.; Rollefson, G.K.

    1958-11-18

    The recovery of plutonium ions from neutron irradiated uranium can be accomplished by bufferlng an aqueous solutlon of the irradiated materials containing tetravalent plutonium to a pH of 4 to 7, adding sufficient acetate to the solution to complex the uranyl present, adding ferric nitrate to form a colloid of ferric hydroxide, plutonlum, and associated fission products, removing and dissolving the colloid in aqueous nitric acid, oxldizlng the plutonium to the hexavalent state by adding permanganate or dichromate, treating the resultant solution with ferric nitrate to form a colloid of ferric hydroxide and associated fission products, and separating the colloid from the plutonlum left in solution.

  6. Progress on plutonium stabilization

    Energy Technology Data Exchange (ETDEWEB)

    Hurt, D. [Defense Nuclear Facilities Safety Board, Washington, DC (United States)

    1996-05-01

    The Defense Nuclear Facilities Safety Board has safety oversight responsibility for most of the facilities where unstable forms of plutonium are being processed and packaged for interim storage. The Board has issued recommendations on plutonium stabilization and has has a considerable influence on DOE`s stabilization schedules and priorities. The Board has not made any recommendations on long-term plutonium disposition, although it may get more involved in the future if DOE develops plans to use defense nuclear facilities for disposition activities.

  7. Surplus yeast tank failing catastrophically

    DEFF Research Database (Denmark)

    Hedlund, Frank Huess

    2016-01-01

    GOOD REASON FOR CAUTION I A large surplus yeast tank shot into the air leaving the floor plate and the contents behind. Although not designed for overpressure, the tank was kept at “very slight overpressure” to suppress nuisance foaming. The brewery was unaware of the hazards of compressed air. T....... The accident described in this article serves to illustrate that care should be taken if a tank originally designed for atmospheric pressure is modified to operate at slight overpressure.......GOOD REASON FOR CAUTION I A large surplus yeast tank shot into the air leaving the floor plate and the contents behind. Although not designed for overpressure, the tank was kept at “very slight overpressure” to suppress nuisance foaming. The brewery was unaware of the hazards of compressed air...

  8. An improved rotating disc cathode cell for electrodeposition of actinides. The case of plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Becerril, V.A.; Tejera, R.A. (Inst. Nacional de Investigaciones Nucleares, Mexico City (Mexico)); Meas, V.Y. (Univ. Autonoma Metropolitana Iztapalapa, Area de Electroquimica, Mexico City (Mexico) CIDETEQ, Queretaro (Mexico)); Ozil, P. (CREMGP, ENSEEG, 38 - Saint Martin d' Heres (France))

    1993-05-01

    An electrolytic rotating disc electrode cell for electrodeposition of very thin and uniform plutonium (Pu) films with consistently high recoveries, was designed. It was made emphasizing the hydrodynamic conditions to be fulfilled by the device in agreement with the rotating disc electrode (RDE) model. The system was characterized by hydrodynamical parameters. The electrodeposition technique will be discussed elsewhere. The deposition yield was 97.5[+-]2.5%. The high quality of the very thin and uniform Pu deposits allowed one to obtain very suitable Pu sources (FWHM=10.8 keV, LM=100 and uniformity =10%) for alpha spectroscopy and for alpha emission probabilities and isotopic ratios studies. (orig.).

  9. Thermodynamic properties of the cubic plutonium hydride solid solution

    Energy Technology Data Exchange (ETDEWEB)

    Haschke, J M

    1981-12-01

    Pressure, temperature, and composition data for the cubic solid solution plutonium hydride phase, PuH/sub x/, have been measured by microbalance methods. Integral enthalpies and entropies of formation have been evaluated for the composition range 1.90 less than or equal to X less than or equal to 3.00. At 550/sup 0/K, ..delta..H/sup 0/ /sub f/(PuH/sub x/(s)) varies linearly from approximately (-38 +- 1) kcal mol/sup -1/ at PuH/sub 190/ to (-50 +- 1 kcal mol/sup -1/) at PuH/sub 3/ /sub 00/. Thermochemical values obtained by reevaluating tensimetric data from the literature are in excellent agreement with these results. Isotopic effects have been quantified by comparing the results for hydride and deuteride, and equations are presented for predicting ..delta..H/sup 0/ /sub f/ and ..delta..S/sup 0/ /sub f/ values for PuH/sub x/(s) and PuD/sub x/(s).

  10. The behaviour of Eu, Pu, Am radionuclide at burning radioactive graphite in an oxygen atmosphere. Computer experiments

    Directory of Open Access Journals (Sweden)

    Kolbin T.S.

    2015-01-01

    Full Text Available Be means of the method of computer thermodynamic simulation we studied the behaviour of the europium, plutonium and americium from the combustion of radioactive graphite in oxygen. Europe is in the form of condensed EuOCl, Eu2O3 and vapour EuO. Pluto is in the form of condensed vapour PuO2 and PuO2. Americium is a condensed AmO2, Am2O3 and vapour Am. The basic reactions occurring compounds with europium, plutonium and americium. Equilibrium constants of the reactions have been determined.

  11. Development of the Plutonium-DTPA Biokinetic Model.

    Science.gov (United States)

    Konzen, Kevin; Brey, Richard

    2015-06-01

    Estimating radionuclide intakes from bioassays following chelation treatment presents a challenge to the dosimetrist due to the observed excretion enhancement of the particular radionuclide of concern where no standard biokinetic model exists. This document provides a Pu-DTPA biokinetic model that may be used for making such determination for plutonium intakes. The Pu-DTPA biokinetic model is intended to supplement the standard recommended biokinetic models. The model was used to evaluate several chelation strategies that resulted in providing recommendations for effective treatment. These recommendations supported early treatment for soluble particle inhalations and an initial 3-day series of DTPA treatments for wounds. Several late chelation strategies were also compared where reduced treatment frequencies proved to be as effective as multiple treatments. The Pu-DTPA biokinetic model can be used to assist in estimating initial intakes of transuranic radionuclides and for studying the effects of different treatment strategies.

  12. A Method for Continuous (239)Pu Determinations in Arctic and Antarctic Ice Cores.

    Science.gov (United States)

    Arienzo, M M; McConnell, J R; Chellman, N; Criscitiello, A S; Curran, M; Fritzsche, D; Kipfstuhl, S; Mulvaney, R; Nolan, M; Opel, T; Sigl, M; Steffensen, J P

    2016-07-05

    Atmospheric nuclear weapons testing (NWT) resulted in the injection of plutonium (Pu) into the atmosphere and subsequent global deposition. We present a new method for continuous semiquantitative measurement of (239)Pu in ice cores, which was used to develop annual records of fallout from NWT in ten ice cores from Greenland and Antarctica. The (239)Pu was measured directly using an inductively coupled plasma-sector field mass spectrometer, thereby reducing analysis time and increasing depth-resolution with respect to previous methods. To validate this method, we compared our one year averaged results to published (239)Pu records and other records of NWT. The (239)Pu profiles from the Arctic ice cores reflected global trends in NWT and were in agreement with discrete Pu profiles from lower latitude ice cores. The (239)Pu measurements in the Antarctic ice cores tracked low latitude NWT, consistent with previously published discrete records from Antarctica. Advantages of the continuous (239)Pu measurement method are (1) reduced sample preparation and analysis time; (2) no requirement for additional ice samples for NWT fallout determinations; (3) measurements are exactly coregistered with all other chemical, elemental, isotopic, and gas measurements from the continuous analytical system; and (4) the long half-life means the (239)Pu record is stable through time.

  13. Thermophysical properties of α−Pu{sub 2}O{sub 3}: A new potential model

    Energy Technology Data Exchange (ETDEWEB)

    Günay, S. D., E-mail: sdgunay@gmail.com; Akdere, Ü.; Taşseven, Ç. [Department of Physics, Faculty of Science, Yildiz Technical University, Davutpaþa Campus, Esenler, 34210, Istanbul (Turkey); Akgenç, B., E-mail: berna.akgenc@kirklareli.edu.tr [Kýrklareli University Department of Physics, Faculty of Science, Kavaklý, 39060, Kýrklareli (Turkey)

    2013-12-16

    α−Pu{sub 2}O{sub 3} is an important material among plutonium based materials in nuclear industry. Pure plutonium surfaces quickly oxidizes into α−Pu{sub 2}O{sub 3} and PuO{sub 2} which are in the form of layers one on another. Here we have investigated thermal properties of α−Pu{sub 2}O{sub 3} by molecular dynamics simulation by using a partially ionic semi-empirical rigid ion potential. Mechanical properties, thermal expansion, and heat capacity are calculated. Results were compared with available experimental data and quantum calculation [2]. Due to the experimental limitations such as toxicity and radiation effects, studying the physical properties of such materials from molecular dynamics simulations have vital importance.

  14. 78 FR 1848 - Plutonium-238 Production for Radioisotope Power Systems for National Aeronautics and Space...

    Science.gov (United States)

    2013-01-09

    ... Plutonium-238 Production for Radioisotope Power Systems for National Aeronautics and Space Administration...-238 (Pu-238) for radioisotope power systems (RPSs) to support the National Aeronautics and Space... Radioisotope Power Systems (Draft Consolidation EIS) in 2005 to consolidate the nuclear operations related...

  15. Nature of non-magnetic strongly-correlated state in delta-plutonium

    NARCIS (Netherlands)

    Pourovskii, L.V.; Katsnelson, M.I.; Lichtenstein, A.I.; Havela, L.; Gouder, T.; Wastin, F.; Shick, A.B.; Drchal, V.; Lander, G.H.

    2006-01-01

    Ab initio relativistic dynamical mean-field theory is applied to resolve the longstanding controversy between theory and experiment in the "simple" face-centered cubic phase of plutonium called delta-Pu. In agreement with experiment, neither static nor dynamical magnetic moments are predicted. In ad

  16. Plutonium emission from the Fukushima accident

    Energy Technology Data Exchange (ETDEWEB)

    Bossew, P., E-mail: pbossew@bfs.de [German Federal Office for Radiation Protection, Berlin (Germany)

    2013-07-01

    A strong earthquake and subsequent tsunami on 11{sup th} March 2011 initiated a severe accident in units 1 to 4 of Fukushima Dai-ichi nuclear power plant, resulting in substantial releases of radionuclides. While much has since been published 00 environmental contamination and exposure to radio--iodine and radio-caesium, little is known about releases of plutonium and other non-volatile elements. Although the total activities of released {sup 131}I, {sup 134}Cs and {sup 137}Cs are of the same order of magnitude as of the Chernobyl accident in 1986, the contribution of little volatile elements, including Pu, is much smaller in Fukushima fallout. The reason is the different physical nature of the accident sequence which led to a release of some 10{sup -}5% of the core inventories only (to be compared with 3.5% from Chernobyl). In this contribution the available data on Pu in Fukushima fallout will be reviewed. Data sources are mainly reports and press releases by Japanese authorities and a few scientific articles. The mean ratio {sup 239+240}Pu: {sup 137}Cs in the near field around the NPP (mainly part of Fukushima prefecture and districts of adjacent prefectures) can be assumed about 3 x 10{sup -}7{sup ,} to be compared to nearly 0.01 in the vicinity of Chernobyl, down to about 3 x 10 {sup -6} in Central Europe. Isotopic ratios {sup 238}Pu: {sup 239+240} Pu are about 2.2 (0.46 and 0.035 in Chemobyl and global fallout, respectively). Activity concentrations of Fukushima- {sup 239+240} Pu in surface soil were found up to above 0.1 Bq/kg d.m. in the immediate vicinity of the Fukushima NPP and about one order of magnitude less in Fukushima city, about 60 km away. The {sup 239+240} Pu activity released into the atmosphere is roughly estimated some 10{sup 9} Bq (Chemobyl : almost 10{sup 14} Bq). (author)

  17. Hematological responses after inhaling {sup 238}PuO{sub 2}: An extrapolation from beagle dogs to humans

    Energy Technology Data Exchange (ETDEWEB)

    Scott, B.R.; Muggenburg, B.A.; Welsh, C.A.; Angerstein, D.A.

    1994-11-01

    The alpha emitter plutonium-238 ({sup 238}Pu), which is produced in uranium-fueled, light-water reactors, is used as a thermoelectric power source for space applications. Inhalation of a mixed oxide form of Pu is the most likely mode of exposure of workers and the general public. Occupational exposures to {sup 238}PuO{sub 2} have occurred in association with the fabrication of radioisotope thermoelectric generators. Organs and tissue at risk for deterministic and stochastic effects of {sup 238}Pu-alpha irradiation include the lung, liver, skeleton, and lymphatic tissue. Little has been reported about the effects of inhaled {sup 238}PuO{sub 2} on peripheral blood cell counts in humans. The purpose of this study was to investigate hematological responses after a single inhalation exposure of Beagle dogs to alpha-emitting {sup 238}PuO{sub 2} particles and to extrapolate results to humans.

  18. Characterization of plutonium-bearing wastes by chemical analysis and analytical electron microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Behrens, R.G. [Los Alamos National Lab., NM (United States); Buck, E.C.; Dietz, N.L.; Bates, J.K.; Van Deventer, E.; Chaiko, D.J. [Argonne National Lab., IL (United States)

    1995-09-01

    This report summarizes the results of characterization studies of plutonium-bearing wastes produced at the US Department of Energy weapons production facilities. Several different solid wastes were characterized, including incinerator ash and ash heels from Rocky Flats Plant and Los Alamos National Laboratory; sand, stag, and crucible waste from Hanford; and LECO crucibles from the Savannah River Site. These materials were characterized by chemical analysis and analytical electron microscopy. The results showed the presence of discrete PuO{sub 2}PuO{sub 2{minus}x}, and Pu{sub 4}O{sub 7} phases, of about 1{mu}m or less in size, in all of the samples examined. In addition, a number of amorphous phases were present that contained plutonium. In all the ash and ash heel samples examined, plutonium phases were found that were completely surrounded by silicate matrices. Consequently, to achieve optimum plutonium recovery in any chemical extraction process, extraction would have to be coupled with ultrafine grinding to average particle sizes of less than 1 {mu}m to liberate the plutonium from the surrounding inert matrix.

  19. BIOLOGICALLY-MEDIATED REMOVAL AND RECOVERY OF PLUTONIUM FROM CONTAMINATED SOIL

    Energy Technology Data Exchange (ETDEWEB)

    Jerger, Douglas E., Ph.D.,; Alperin, Edward S., QEP,; Holmes, Robert G., Ph.D.

    2003-02-27

    An innovative biological treatment technology successfully reduced plutonium concentration in soil from the Nevada Test Site (NTS) by over 80%. The final volume of plutonium-contaminated material that required disposal was reduced by over 90%. These results, achieved by an independent testing laboratory, confirm the results reported previously using NTS soil. In the previous test a 2530-gram sample of soil (350 to 400 pCi/g Pu) resulted in production of 131 grams of sludge (6,320 pCi/ g Pu) and a treated soil containing 72 pCi/g of Pu. The technology is based on the biological acidification of the soil and subsequent removal of the plutonium and other dissolved metals by a low volume, low energy water leaching process. The leachate is treated in a sulfate-reducing bioreactor to precipitate the metals as metal sulfides. Water may be recycled as process water or disposed since the treatment process removes over 99% of the dissolved metals including plutonium from the water. The plutonium is contained as a stable sludge that can be containerized for final disposal. Full-scale process costs have been developed which employ widely used treatment technologies such as aerated soil piles (biopiles) and bioreactors. The process costs were less than $10 per cubic foot, which were 40 to 50% lower than the baseline costs for the treatment of the NTS soil. The equipment and materials for water and sludge treatment and soil handling are commercially available.

  20. Symbiotic Pu/Th fuel cycle for HTGR

    Energy Technology Data Exchange (ETDEWEB)

    Girardi, Enrico; Lecarpentier, David [EDF R and D, Les Renardieres, 77818 Moret sur Loing cedex (France)

    2006-07-01

    HTGRs, loaded with uranium or plutonium fuel do not authorize high breeding ratios. Consequently, the Gen IV requirement of sustainability with respect to the use of fissile resources may be difficult to meet. Relying on the thorium conversion into fissile uranium 233, the use of thorium is promising regarding the breeding ratio. Accordingly, the symbiotic Pu/Th fuel cycle is an interesting way to optimize the energetic use of plutonium. In the first part of this paper, we compare the performances of HTRs with different types of fuel (15% enriched U, Pu alone, Th-Pu) on the resource consumption. Relying on HTGRs, a good conversion ratio (typically 0.8) is mandatory to satisfy high temperature needs in the long term. In the second part, we discuss the neutronic calculation scheme for a prismatic HTGR annular core (GTMHR like, with an internal graphite reflector), and for a large HTGR (modeled with an assembly calculation). In the last part of the paper, Pu/Th, U233/Th and Pu-U233/Th fuel cycle are studied for the two types of HTGRs. The performances in terms of conversion ratios are compared. For a given power of 300 Mwe, several compositions for the fuel are studied. The fraction of thorium in the fuel composition is varying from 0% to 99% and the total fuel mass charged in the core ranges from 1200 kg to 15,000 kg. We show that good conversion ratios are very difficult to obtain for annular HTGRs. New designs must be considered, with a larger core, and a smaller power density (to reach the passive evacuation of residual power). Finally, a preliminary strategy for the deployment of these fuel cycles is presented. (authors)

  1. Radionuclide release from irradiated Th-Pu mox fuel

    Energy Technology Data Exchange (ETDEWEB)

    Rodriguez, N.; Quinones, J. [Ciemat., Avda. Complutense 22. E-28040 Madrid (Spain); Cobos, J. [Centro Nacional de Aceleradores, Parque Tecnologico Cartuja 93, Av. Thomas Alva Edison, 7, E-41092 Sevilla (Spain); Rondinella, V.V.; Van Winckel, S.; Somers, J.; Papaioanu, D.; Glatz, J.P. [European Commission, Joint Research Centre, Institute for Transuranium Elements, Postfach 2340, D-76125 Karlsruhe (Germany)

    2010-07-01

    Plutonium and minor actinides produced as by-products of the UO{sub 2} nuclear cycle could be considered as waste or energy source depending on the strategy selected in the nuclear energy programme. Considering Pu and Minor Actinides as a source, they can be burned in existing water reactor for diminishing the radiotoxicity of the spent fuel, it is necessary to use 'inactive' materials as matrix like ThO{sub 2}. ThO{sub 2} matrix has demonstrated its Pu burning efficiency and higher corrosion resistance than UO{sub 2}. Uranium-plutonium mixed oxide (MOX) fuel efficiency is low because the presence of U in MOX results in the creation of some new Pu under irradiation. The dissolution behaviour of irradiated (Th,Pu)O{sub 2} pellets with burn-up of 38.8 MWd/kg Th has been studied in carbonated (20 mM HCO{sub 3}{sup -}), deionised and granite ground water solution in a hot cell. The dissolution behaviour of Th, Pu, U and Np was studied in order to find out whether radionuclides release is depending on the matrix dissolution (solubility control). After irradiating the samples, K-ORIGEN and ORIGEN ARP codes were used to find out the theoretical inventory. Afterwards, fuel samples were dissolved completely and analyzed, in order to determine the experimental radionuclide inventory of the irradiated fuel. Th matrix alteration appears to reach an steady state and radionuclides dissolution shows dependence on the matrix behaviour as can be observed through the FIAP results. (authors)

  2. Plutonium dissolution process

    Science.gov (United States)

    Vest, Michael A.; Fink, Samuel D.; Karraker, David G.; Moore, Edwin N.; Holcomb, H. Perry

    1996-01-01

    A two-step process for dissolving plutonium metal, which two steps can be carried out sequentially or simultaneously. Plutonium metal is exposed to a first mixture containing approximately 1.0M-1.67M sulfamic acid and 0.0025M-0.1M fluoride, the mixture having been heated to a temperature between 45.degree. C. and 70.degree. C. The mixture will dissolve a first portion of the plutonium metal but leave a portion of the plutonium in an oxide residue. Then, a mineral acid and additional fluoride are added to dissolve the residue. Alteratively, nitric acid in a concentration between approximately 0.05M and 0.067M is added to the first mixture to dissolve the residue as it is produced. Hydrogen released during the dissolution process is diluted with nitrogen.

  3. Separation Of Uranium And Plutonium Isotopes For Measurement By Multi Collector Inductively Coupled Plasma Mass Spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Martinelli, R E; Hamilton, T F; Williams, R W; Kehl, S R

    2009-03-29

    Uranium (U) and plutonium (Pu) isotopes in coral soils, contaminated by nuclear weapons testing in the northern Marshall Islands, were isolated by ion-exchange chromatography and analyzed by mass spectrometry. The soil samples were spiked with {sup 233}U and {sup 242}Pu tracers, dissolved in minerals acids, and U and Pu isotopes isolated and purified on commercially available ion-exchange columns. The ion-exchange technique employed a TEVA{reg_sign} column coupled to a UTEVA{reg_sign} column. U and Pu isotope fractions were then further isolated using separate elution schemes, and the purified fractions containing U and Pu isotopes analyzed sequentially using multi-collector inductively coupled plasma mass spectrometer (MCICP-MS). High precision measurements of {sup 234}U/{sup 235}U, {sup 238}U/{sup 235}U, {sup 236}U/{sup 235}U, and {sup 240}Pu/{sup 239}Pu in soil samples were attained using the described methodology and instrumentation, and provide a basis for conducting more detailed assessments of the behavior and transfer of uranium and plutonium in the environment.

  4. High-Precision Plutonium Isotopic Compositions Measured on Los Alamos National Laboratory’s General’s Tanks Samples: Bearing on Model Ages, Reactor Modelling, and Sources of Material. Further Discussion of Chronometry

    Energy Technology Data Exchange (ETDEWEB)

    Spencer, Khalil J. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rim, Jung Ho [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Porterfield, Donivan R. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Roback, Robert Clifford [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Boukhalfa, Hakim [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Stanley, Floyd E. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

    2015-06-29

    In this study, we re-analyzed late-1940’s, Manhattan Project era Plutonium-rich sludge samples recovered from the ''General’s Tanks'' located within the nation’s oldest Plutonium processing facility, Technical Area 21. These samples were initially characterized by lower accuracy, and lower precision mass spectrometric techniques. We report here information that was previously not discernable: the two tanks contain isotopically distinct Pu not only for the major (i.e., 240Pu, 239Pu) but trace (238Pu ,241Pu, 242Pu) isotopes. Revised isotopics slightly changed the calculated 241Am-241Pu model ages and interpretations.

  5. Plutonium, Mineralogy and Radiation Effects

    Science.gov (United States)

    Ewing, R. C.

    2006-05-01

    During the past fifty years, more than 1,800 metric tonnes of Pu and substantial quantities of other "minor" actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranic elements can be a source of energy in fission reactions (e.g., 239Pu), a source of fissile material for nuclear weapons (e.g., 239Pu and 237Np), or are of environmental concern because of their long half- lives and radiotoxicity (e.g., 239Pu, t1/2 = 24,100 years, and 237Np, t1/2 = 2.1 million years). There are two basic strategies for the disposition of these elements: 1.) to "burn" or transmute the actinides using nuclear reactors or accelerators; 2.) to "sequester" the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, such as zircon or isometric pyrochlore, A2B2O7 (A = rare earths; B = Ti, Zr, Sn, Hf; Fd3m; Z=8), for the immobilization of actinides, particularly plutonium. One of the principal concerns has been the accumulation of structural damage caused by alpha-decay events, particularly from the recoil nucleus. Systematic ion beam irradiation studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high fluences of alpha-decay event damage. Some compositions, Gd2Ti2O7, are amorphized at relatively low doses (0.2 displacements per atom, dpa, at room temperature), while other compositions, Gd2Zr2O7, do not amorphize (even at doses of > 40 dpa at 25K), but instead disorder to a defect fluorite structure. By changing the composition of the A-site (e.g., substitution of different rare earth elements), the temperature above which the pyrochlore composition can no longer be amorphized, Tc, varies by >600 K (e.g., Lu2Ti2O7: Tc = 480 K; Gd2Ti2O7: Tc = 1120 K). The variation in response to irradiation as a function of composition can be used to model the long

  6. Pu-239 and Pu-240 inventories and Pu-240/ Pu-239 atom ratios in the water column off Sanriku, Japan.

    Science.gov (United States)

    Yamada, Masatoshi; Zheng, Jian; Aono, Tatsuo

    2013-04-01

    A magnitude 9.0 earthquake and subsequent tsunami occurred in the Pacific Ocean off northern Honshu, Japan, on 11 March 2011 which caused severe damage to the Fukushima Dai-ichi Nuclear Power Plant. This accident has resulted in a substantial release of radioactive materials to the atmosphere and ocean, and has caused extensive contamination of the environment. However, no information is available on the amounts of radionuclides such as Pu isotopes released into the ocean at this time. Investigating the background baseline concentration and atom ratio of Pu isotopes in seawater is important for assessment of the possible contamination in the marine environment. Pu-239 (half-life: 24,100 years), Pu-240 (half-life: 6,560 years) and Pu-241 (half-life: 14.325 years) mainly have been released into the environment as the result of atmospheric nuclear weapons testing. The atom ratio of Pu-240/Pu-239 is a powerful fingerprint to identify the sources of Pu in the ocean. The Pu-239 and Pu-240 inventories and Pu-240/Pu-239 atom ratios in seawater samples collected in the western North Pacific off Sanriku before the accident at Fukushima Dai-ichi Nuclear Power Plant will provide useful background baseline data for understanding the process controlling Pu transport and for distinguishing additional Pu sources. Seawater samples were collected with acoustically triggered quadruple PVC sampling bottles during the KH-98-3 cruise of the R/V Hakuho-Maru. The Pu-240/Pu-239 atom ratios were measured with a double-focusing SF-ICP-MS, which was equipped with a guard electrode to eliminate secondary discharge in the plasma and to enhance overall sensitivity. The Pu-239 and Pu-240 concentrations were 2.07 and 1.67 mBq/m3 in the surface water, respectively, and increased with depth; a subsurface maximum was identified at 750 m depth, and the concentrations decreased with depth, then increased at the bottom layer. The total Pu-239+240 inventory in the entire water column (depth interval 0

  7. Analysis of the effects of inter-individual variation in the distribution of plutonium in skeleton and liver.

    Science.gov (United States)

    Klein, W; Breustedt, B

    2014-01-01

    One important parameter for biokinetic plutonium modelling is the ratio between the contents of plutonium in liver and skeleton. Autopsy data show a vast inter-individual variation in the partitioning between these organs. The capacity of recent biokinetic models for plutonium to reproduce these variations was studied. Autopsy data for plutonium amounts in liver and skeleton for both (238)Pu and (239)Pu isotopes can be merged into a single data set following several statistical tests. Simulations with different parameter values generate a mapping between the autopsy values and the model parameters. The observed partitioning distribution can be transformed into a distribution of transfer rates, which would result in the observed data. Besides, the variation in the partitioning between liver and skeleton leads via biliary pathway to a variation in the excretion ratio. This can be used to estimate an individual partitioning factor, which can be used in individual case assessments.

  8. Neutron monitoring of plutonium at the ZPPR storage vault

    Energy Technology Data Exchange (ETDEWEB)

    Caldwell, J.T.; Kuckertz, T.H.; Bieri, J.M.; France, S.W.; Goin, R.W.; Hastings, R.D.; Pratt, J.C.; Shunk, E.R.

    1981-12-01

    We investigated a method for monitoring a typical large storage vault for unauthorized removal of plutonium. The method is based on the assumption that the neutron field in a vault produced by a particular geometric configuration of bulk plutonium remains constant in time and space as long as the configuration is undisturbed. To observe such a neutron field, we installed an array of 25 neutron detectors in the ceiling of a plutonium storage vault at Argonne National Laboratory West. Each neutron detector provided an independent spatial measurement of the vault neutron field. Data collected by each detector were processed to determine whether statistically significant changes had occurred in the neutron field. Continuous observation experiments measured the long-term stability of the system. Removal experiments were performed in which known quantities of plutonium were removed from the vault. Both types of experiments demonstrated that the neutron monitoring system can detect removal or addition of bulk plutonium (11% /sup 240/Pu) whose mass is as small as 0.04% of the total inventory.

  9. RAPID DETERMINATION OF 237 NP AND PU ISOTOPES IN WATER BY INDUCTIVELY COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY

    Energy Technology Data Exchange (ETDEWEB)

    Maxwell, S.; Jones, V.; Culligan, B.; Nichols, S.; Noyes, G.

    2010-06-23

    A new method that allows rapid preconcentration and separation of plutonium and neptunium in water samples was developed for the measurement of {sup 237}Np and Pu isotopes by inductively-coupled plasma mass spectrometry (ICP-MS) and alpha spectrometry; a hybrid approach. {sup 238}U can interfere with {sup 239}Pu measurement by ICP-MS as {sup 238}UH{sup +} mass overlap and {sup 237}Np via peak tailing. The method provide enhanced removal of uranium by separating Pu and Np initially on TEVA Resin, then moving Pu to DGA resin for additional removal of uranium. The decontamination factor for uranium from Pu is almost 100,000 and the decontamination factor for U from Np is greater than 10,000. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration is performed using a streamlined calcium phosphate precipitation method. Purified solutions are split between ICP-MS and alpha spectrometry so that long and short-lived Pu isotopes can be measured successfully. The method allows for simultaneous extraction of 20 samples (including QC samples) in 4 to 6 hours, and can also be used for emergency response. {sup 239}Pu, {sup 242}Pu and {sup 237}Np were measured by ICP-MS, while {sup 236}Pu, {sup 238}Pu, and {sup 239}Pu were measured by alpha spectrometry.

  10. Analytical method for the determination of Np and Pu in sea water by AMS with respect to the Fukushima accident

    Energy Technology Data Exchange (ETDEWEB)

    Hain, K., E-mail: karin.hain@mytum.de [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Faestermann, T.; Famulok, N.; Fimiani, L.; Gómez-Guzmán, J.M.; Korschinek, G. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Kortmann, F.; Lierse von Gostomski, Ch. [Radiochemie München, Technische Universität München, Walther-Meißner-Str.3, 85748 Garching (Germany); Ludwig, P. [Physics Department, Technische Universität München, James-Franck-Str.1, 85748 Garching (Germany); Shinonaga, T. [Helmholtz Zentrum München, German Research Center for Environmental Health, Institute of Radiation Protection, Ingolstädter Landstrasse 1, 855764 Neuherberg (Germany)

    2015-10-15

    A chemical separation procedure for plutonium (Pu) and neptunium (Np) was developed using extraction chromatography, mass spectrometry and radiometric analysis to determine their concentrations and isotopic ratios in sea water. {sup 241}Am, which causes isobaric background to {sup 241}Pu in mass spectrometric measurements, was successfully separated from the Pu fraction by this method. Water samples which were spiked with {sup 242}Pu and {sup 237}Np or {sup 239}Np, respectively, were used for chemical yield determination. The chemical yields of Pu and Np, which were determined by alpha and gamma spectrometry at the Radiochemie München (RCM), of more than 85% were obtained. The developed method was applied to analyze the concentration of Pu and Np in the certified reference material, IAEA-443, by Accelerator Mass Spectrometry (AMS) at the Maier–Leibnitz-Laboratory (MLL) to check the applicability of the method to sea water samples. The concentrations of {sup 240}Pu, {sup 241}Pu and {sup 237}Np obtained in this study are in agreement with the certified and literature values within the uncertainties. Due to strong isotopic interference of {sup 239}Pu with {sup 238}U, it was not possible to analyze the concentration of {sup 239}Pu. Some modifications of the chemical separation method to suppress the uranium (U) fraction are under consideration. This method can be used for the analysis of Pu and Np in Pacific Ocean water samples collected after the Fukushima accident.

  11. Glutarimidedioxime. A complexing and reducing reagent for plutonium recovery from spent nuclear fuel reprocessing

    Energy Technology Data Exchange (ETDEWEB)

    Xian, Liang [China Institute of Atomic Energy, Beijing (China). Radiochemistry Dept.; Tian, Guoxin [China Institute of Atomic Energy, Beijing (China). Radiochemistry Dept.; Lawrence Berkeley National Laboratory, Berkeley, CA (United States). Chemical Sciences Div.; Beavers, Christine M.; Teat, Simon J. [Lawrence Berkeley National Laboratory, Berkeley, CA (United States). Advanced Light Source; Shuh, David K. [Lawrence Berkeley National Laboratory, Berkeley, CA (United States). Chemical Sciences Div.

    2016-04-04

    Efficient separation processes for recovering uranium and plutonium from spent nuclear fuel are essential to the development of advanced nuclear fuel cycles. The performance characteristics of a new salt-free complexing and reducing reagent, glutarimidedioxime (H{sub 2}A), are reported for recovering plutonium in a PUREX process. With a phase ratio of organic to aqueous of up to 10:1, plutonium can be effectively stripped from 30 % tributyl phosphate (TBP) in kerosene into 1M HNO{sub 3} with H{sub 2}A. The complexation-reduction mechanism is illustrated with the combination of UV/Vis absorption spectra and the crystal structure of a Pu{sup IV} complex with the reagent. The fast stripping rate and the high efficiency for stripping Pu{sup IV}, through the complexation-reduction mechanism, is suitable for use in centrifugal contactors with very short contact/resident times, thereby offering significant advantages over conventional processes.

  12. X-ray absorption fine structure spectroscopy of plutonium complexes with bacillus sphaericus

    Energy Technology Data Exchange (ETDEWEB)

    Panak, P.J.; Booth, C.H.; Caulder, D.L.; Bucher, J.J.; Shuh, D.K. [Lawrence Berkeley National Lab. (LBNL), Chemical Sciences Div., The Glenn T. Seaborg Center, Berkeley, CA (United States); Nitsche, H. [Lawrence Berkeley National Lab. (LBNL), Chemical Sciences Div., The Glenn T. Seaborg Center, Berkeley, CA (United States); Univ. of California at Berkeley, Dept. of Chemistry, Berkeley, CA (United States)

    2002-07-01

    Knowledge of the plutonium complexes formed with bacterial cells is critical for predicting the influence of microbial interactions on the migration behavior of actinides in the environment. This investigation describes the interaction of plutonium(VI) with cells of the aerobic soil bacteria, Bacillus sphaericus. The studies include the quantification of carboxylate and phosphate functional groups on the cell walls by potentiometric titration and the determination of the plutonium speciation by X-ray absorption fine structure (XAFS). Extended-XAFS (EXAFS) was used to determine the identity of the Pu(VI) interfacial complex with the bacteria, and the Pu(VI) was found primarily bound to phosphate groups on the cell surface. No carboxylate complexation was detected. (orig.)

  13. Investigation of environmental samples from Fukushima with respect to uranium and plutonium by AMS; Untersuchung von Umweltproben aus Fukushima in Bezug auf Plutonium und Uran mittels AMS

    Energy Technology Data Exchange (ETDEWEB)

    Schneider, Stephanie

    2017-02-01

    In March 2011, the nuclear power plant Fukushima Dai-ichi was seriously damaged by a tsunami caused by an earthquake. During the accident large quantities of radionuclides, mainly of the volatile elements cesium and iodine, were released to the environment. In small amounts refractory elements such as plutonium and uranium have also been released. Plutonium and the uraniumisotope {sup 236}U have primarily been delivered by human activities in the environment. Large amounts were released during the atmospheric nuclear weapons tests. Additional sources are accidents in nuclear facilities, like Chernobyl. Every source has its own characteristic isotopic composition. It is therefore possible to determine the origin of the contamination by measuring the isotopic ratios of {sup 240}Pu/{sup 239}Pu and {sup 236}U/{sup 238}U. These ratios can be determined by using accelerator mass spectrometry. Due to its high sensitivity, it is possible to measure even small amounts of plutonium and especially of {sup 236}U. These measurements were performed using the compact 500 kV facility ''TANDY'' of ETH Zurich. In 2013 and 2015 vegetation, litter and soil drill core samples were taken in the contaminated area in Fukushima prefecture. In 2015 samples were taken as close to the sampling locations of the 2013 campaign as possible. After isolation of plutonium and uranium by chemical extraction, separate targets were prepared for the measurement. The {sup 240}Pu/{sup 239}Pu ratios indicate global fallout as the plutonium source for most samples. The plutonium of the reactors of Fukushima Dai-ichi is located in the upper layers like in vegetation or litter. From the uranium ratios alone the reactors could not unambigously be identified as the source of {sup 236}U. However, this is plausible in the cases were reactor plutonium was detected. None of the samples contained higher plutonium activity concentrations than in the rest of Japan, caused by global fallout. This

  14. On the Burning of Plutonium Originating from Light Water Reactor Use in a Fast Molten Salt Reactor—A Neutron Physical Study

    Directory of Open Access Journals (Sweden)

    Bruno Merk

    2015-11-01

    Full Text Available An efficient burning of the plutonium produced during light water reactor (LWR operation has the potential to significantly improve the sustainability indices of LWR operations. The work offers a comparison of the efficiency of Pu burning in different reactor configurations—a molten salt fast reactor, a LWR with mixed oxide (MOX fuel, and a sodium cooled fast reactor. The calculations are performed using the HELIOS 2 code. All results are evaluated against the plutonium burning efficiency determined in the Consommation Accrue de Plutonium dans les Réacteurs à Neutrons RApides (CAPRA project. The results are discussed with special view on the increased sustainability of LWR use in the case of successful avoidance of an accumulation of Pu which otherwise would have to be forwarded to a final disposal. A strategic discussion is given about the unavoidable plutonium production, the possibility to burn the plutonium to avoid a burden for the future generations which would have to be controlled.

  15. Physical and economical aspects of Pu multiple recycling on the basis of REMIX reprocessing technology in thermal reactors

    Directory of Open Access Journals (Sweden)

    Teplov Pavel S.

    2016-01-01

    Full Text Available The basic strategy of Russian nuclear energy is propagation of a closed fuel cycle on the basis of fast breeder and thermal reactors, as well as the solution of the spent nuclear fuel accumulation and resource problems. The three variants of multiple Pu and U recycling in Russian pressurized water reactor concept reactors on the basis of REgenerated MIXture of U, Pu oxides (REMIX reprocessing technology are considered in this work. The REMIX fuel is fabricated from an unseparated mixture of uranium and plutonium obtained during spent fuel reprocessing with further makeup by enriched natural U or reactor grade Pu. This makes it possible to recycle several times the total amount of Pu obtained from the spent fuel. The main difference in Pu recycling is the concept of 100% or partial fuel loading of the core. The third variant is heterogeneous composition of enriched uranium and uranium–plutonium mixed oxide fuel pins in one fuel assembly. It should be noted that all fuel assemblies with Pu require the involvement of expensive technologies during manufacturing. These three variants of the full core loadings can be balanced on zero Pu accumulation in the cycle. The various physical and economical aspects of Pu and U multiple recycling in selected variants are observed in the given work.

  16. Conversion electron spectrometry of Pu isotopes with a silicon drift detector.

    Science.gov (United States)

    Pommé, S; Paepen, J; Peräjärvi, K; Turunen, J; Pöllänen, R

    2016-03-01

    An electron spectrometry set-up was built at IRMM consisting of a vacuum chamber with a moveable source holder and windowless Peltier-cooled silicon drift detector (SDD). The SDD is well suited for measuring low-energy x rays and electrons emitted from thin radioactive sources with low self-absorption. The attainable energy resolution is better than 0.5keV for electrons of 30keV. It has been used to measure the conversion electron spectra of three plutonium isotopes, i.e. (238)Pu, (239)Pu, (240)Pu, as well as (241)Am (being a decay product of (241)Pu). The obtained mixed x-ray and electron spectra are compared with spectra obtained with a close-geometry set-up using another SDD in STUK and spectra measured with a Si(Li) detector at IRMM. The potential of conversion electron spectrometry for isotopic analysis of mixed plutonium samples is investigated. With respect to the (240)Pu/(239)Pu isotopic ratio, the conversion electron peaks of both isotopes are more clearly separated than their largely overlapping peaks in alpha spectra.

  17. Trend in Plutonium Content of MOX in Thermal Reactor Use and Irradiation Behavior of MOX with High Plutonium Content

    Energy Technology Data Exchange (ETDEWEB)

    Nakae, N.; Baba, T.; Kamimura, K. [Japan Nuclear Energy Safety Organization - JNES, TOKYU REIT Toranomon Bldg., 3-17-1, Toranomon, Minato-ku, Tokyo, 105-0001 (Japan); Verwerft, M.; Jutier, F. [SCK-CEN (Belgium)

    2009-06-15

    The uranium enrichment of UO{sub 2} fuel for the current power reactors, both PWR and BWR, tends to increase because of increasing burn-up target. The plutonium content of MOX fuel used in thermal reactors shall be determined in order to have reactivity worth equivalent to enriched UO{sub 2} fuel based on physical accounting method for adjusting fissile enrichment, thus the plutonium content tends to increase according to the increment of the uranium enrichment of UO{sub 2} fuel and this trend shall further be accentuated due to the fact that Pu recovered from reprocessing of the spent high burnup UO{sub 2} fuel contains less fissile isotopes. The plutonium content is calculated by use of the physical accounting method with the plutonium having several kinds of isotope ratios and the calculation results indicate that the plutonium content in MOX will evolve to ratios in excess of 10%. It shall be, therefore, important to know the irradiation behavior of MOX with high plutonium content of more than 10 wt%. MOX fuel rods having a plutonium content of about 14 wt% and fabricated by use of MIMAS process have been irradiated under PWR conditions in the Belgian test reactors BR-3 and BR-2. The peak fuel rod burn-up of the fuel rods studied in this paper ranges from 31 to 37 GWd/t-HM, and their average burnup is about 22-26 GWd/t-HM with the rod averaged linear heat generation rate of about 15-21 kW/m. The MOX rods are investigated by destructive and non-destructive post irradiation examinations and some of them are now continued to be irradiated in BR-2. Mixed Oxide (U,Pu)O{sub 2} fuel produced by the MIMAS process results in a fine dispersion of Pu enriched particles in a UO{sub 2} matrix and effectively gives three enrichment classes: low, medium and high enriched. The high enriched particles (often called 'Pu spots'), have an enrichment of around 25 wt% Pu, the low enriched phase is the UO{sub 2} matrix and contains only trace amounts of Pu. An

  18. Americium and plutonium in water, biota, and sediment from the central Oregon coast

    Energy Technology Data Exchange (ETDEWEB)

    Nielsen, R. D.

    1982-06-01

    Plutonium-239, 240 and americium-241 were measured in the mussel Mytilus californianus from the region of Coos Bay, OR. The flesh of this species has a plutonium concentration of about 90 fCi/kg, and an Am-241/Pu-239, 240 ratio that is high relative to mixed fallout, ranging between two and three. Transuranic concentrations in sediment, unfiltered water, and filterable particulates were also measured; none of these materials has an Am/Pu ratio as greatly elevated as the mussels, and there is no apparent difference in the Am/Pu ratio of terrestrial runoff and coastal water. Sediment core profiles do not allow accumulation rates or depositional histories to be identified, but it does not appear that material characterized by a high Am/Pu ratio has ever been introduced to this estuary. Other bivalves (Tresus capax and Macoma nasuta) and a polychaete (Abarenicola sp.) do not have an elevated Am/Pu ratio, although the absolute activity of plutonium in the infaunal bivalves is roughly four times that in the mussels.

  19. 钚在地下水中的存在形式及影响因素分析%Analysis on Plutonium Existing Forms and Its Affection Factors in Groundwater

    Institute of Scientific and Technical Information of China (English)

    朵天惠; 王永利; 黄支刚; 蔡兴琪

    2013-01-01

    The existing forms of plutonium in groundwater from a drilling hole in a study region was simulated by the geochemical modeling program PHREEQC. The main conclusions are as follows: the main existing form of plutonium in the groundwater is Pu (Ⅳ ) in Pu (CO3 )2 (OH)22- which take up 82. 28%, the subordination chemical form is Pu (V) as PuO2+, PuO2CO3- and Pu ( Ⅵ) as PuO2 (CO3)22- which take up 8. 52% , 7. 82% and 1. 17% respectively. In additon, the influence of pH and pE value on the existing forms of plutonium was also studied and it was found that pH and pE value have different impacts on the chemical form of plutonium.%运用PHREEQC模拟软件对西北某区钻孔地下水中钚的存在形式进行了模拟计算,结果显示,钚以Pu(Ⅳ)价态的Pu (CO3)2(OH)22-为主,占82.28%;其次为Pu (Ⅴ)价态的PuO2+、PuO2CO3-和Pu(Ⅵ)价态的PuO2 (CO3)22-,分别占8.52%、7.82%和1.17%.同时研究了pH值和pE值对钚在地下水中存在形式的影响.

  20. Chemical thermodynamics of nuclear materials. Pt. 9. The high temperature heat capacity of plutonium-3. 2 at. % gallium alloy

    Energy Technology Data Exchange (ETDEWEB)

    Adams, R.O.; Oetting, F.L. (Rockwell International Corp., Golden, CO (USA). Energy Systems Group)

    The heat capacity of delta-stabilized plutonium (Pu-3.2 at.% Ga) has been determined from 330 to 700 K using an adiabatic calorimeter. It was found that a large portion of the total heat capacity in this temperature range is due to some combination of the electronic heat capacity and the anharmonic heat capacity. By including certain data from the literature, the thermal functions for this plutonium-gallium alloy were calculated in the temperature range 298 to 700 K.

  1. The optimization of an AP1000 fuel assembly for the transmutation of plutonium and minor actinides

    Science.gov (United States)

    Washington, Jeremy A.

    The average nuclear power plant produces twenty metric tons of used nuclear fuel per year, containing approximately 95 wt% uranium, 1 wt% plutonium, and 4 wt% fission products and transuranic elements. Fast reactors are a preferred option for the transmutation of plutonium and minor actinides; however, an optimistic deployment time of at least 20 years indicates a need for a near-term solution. The goal of this thesis is to examine the potential of light water reactors for plutonium and minor actinides transmutation as a near-term solution. This thesis screens the available nuclear isotope database to identify potential absorbers as coatings on a transmutation fuel in a light water reactor. A spectral shift absorber coating tunes the neutron energy spectrum experienced by the underlying target fuel. Eleven different spectral shift absorbers (B4C, CdO, Dy2O3, Er 2O3, Eu2O3, Gd2O3, HfO2, In2O3, Lu2O3, Sm2O3, and TaC) have been selected for further evaluation. A model developed using the NEWT module of SCALE 6.1 code provided performance data for the burnup of the target fuel rods. Irradiation of the target fuels occurs in a Westinghouse 17x17 XL Robust Fuel Assembly over a 1400 Effective Full Power Days (EFPD) interval. The fuels evaluated in this thesis include PuO2, Pu3Si2, PuN, MOX, PuZrH, PuZrHTh, PuZrO 2, and PuUZrH. MOX (5 wt% PuO2), Pu0.31ZrH 1.6Th1.08, and PuZrO2MgO (8 wt%) are selected for detailed analysis in a multi-pin transmutation assembly. A coupled model optimized the resulting transmutation fuel elements. The optimization considered three stages of fuel assemblies containing target fuel pins. The first stage optimized four target fuel pins adjacent to the central instrumentation channel. The second stage evaluated a variety of assemblies with multiple target fuel pins and the third stage re-optimized target fuel pins in the second-stage assembly. A PuZrO2MgO (8 wt%) target fuel with a coating of Lu 2O3 resulted in the greatest reduction in curium-244

  2. Goethite colloid enhanced Pu transport through a single saturated fracture in granite.

    Science.gov (United States)

    Lin, Jianfeng; Dang, Haijun; Xie, Jinchuan; Li, Mei; Zhou, Guoqing; Zhang, Jihong; Zhang, Haitao; Yi, Xiaowei

    2014-08-01

    α-FeOOH, a stable iron oxide in nature, can strongly absorb the low-solubility plutonium (Pu) in aquifers. However, whether Pu transports though a single saturated fracture can be enhanced in the presence of α-FeOOH colloids remains unknown. Experimental studies were carried out to evaluate Pu mobilization at different water flow velocity, as affected by goethite colloids with various concentrations. Goethite nanorods were used to prepare (α-FeOOH)-associated Pu suspensions with α-FeOOH concentration of (0-150) mgL(-1). The work experimentally evidenced that α-FeOOH colloid does enhance transport of Pu through fractured granites. The fraction of mobile (239)Pu (RPu, m=41.5%) associated with the α-FeOOH of an extremely low colloid concentration (0.2mgL(-1)) is much larger than that in absence of α-FeOOH (RPu, m=6.98%). However, plutonium mobility began to decrease when α-FeOOH concentration was increased to 1.0mgL(-1). On the other hand, the fraction of mobile Pu increased gradually with the water flow velocity. Based on the experimental data, the mechanisms underlying the (α-FeOOH)-associated plutonium transport are comprehensively discussed in view of its dynamic deposition onto the granite surfaces, which is decided mainly by the relative interaction between the colloid particle and the immobile surface. This interaction is a balance of electrostatic force (may be repulsive or attractive), the van der Walls force, and the shear stress of flow.

  3. Particulate distribution of plutonium and americium in surface waters from the Spanish Mediterranean coast

    Energy Technology Data Exchange (ETDEWEB)

    Molero, J.; Sanchez-Cabeza, J.A.; Merino, J.; Vidal-Quadras, A. [Universidad Autonoma de Barcelona (Spain); Vives Batlle, J.; Mitchell, P.I. [University Coll., Dublin (Ireland)

    1995-12-31

    Measurements of the particulate distribution of plutonium and americium in Spanish Mediterranean coastal waters have been carried out. Plutonium-239,340 and {sup 241}Am concentrations have been measured in suspended particulate matter by filtering (< 0.22 {mu}m) large volume (200-300 litres) sea water samples. Results indicate that particulate plutonium constitutes on average 11 {+-} 4% of the total concentration in sea water. In the case of americium this percentage rises to 45 {+-} 14%. From the {sup 241}Am/{sup 239,240}Pu activity ratios it is clear that suspended particulate matter is enriched in {sup 241}Am relative to {sup 239,240}Pu by a factor 8 {+-} 4. Plutonium and americium in surface Mediterranean coastal waters appear to be fractionated as they present a different transfer rate to the particles. Our measurements allowed us to estimate sediment-water distribution coefficients (K{sub d}), which are a key parameter to interpret differences between the behaviour of plutonium and americium in sea water. Distribution coefficients K{sub d} have been estimated to be (1.4 {+-} 0.5) x 10{sup 5} litres kg{sup -1} for plutonium and (0.9 {+-} 0.5) x 10{sup 6} litres kg{sup -1} for americium in surface Mediterranean coastal waters. (author).

  4. Developing a physiologically based approach for modeling plutonium decorporation therapy with DTPA.

    Science.gov (United States)

    Kastl, Manuel; Giussani, Augusto; Blanchardon, Eric; Breustedt, Bastian; Fritsch, Paul; Hoeschen, Christoph; Lopez, Maria Antonia

    2014-11-01

    To develop a physiologically based compartmental approach for modeling plutonium decorporation therapy with the chelating agent Diethylenetriaminepentaacetic acid (Ca-DTPA/Zn-DTPA). Model calculations were performed using the software package SAAM II (©The Epsilon Group, Charlottesville, Virginia, USA). The Luciani/Polig compartmental model with age-dependent description of the bone recycling processes was used for the biokinetics of plutonium. The Luciani/Polig model was slightly modified in order to account for the speciation of plutonium in blood and for the different affinities for DTPA of the present chemical species. The introduction of two separate blood compartments, describing low-molecular-weight complexes of plutonium (Pu-LW) and transferrin-bound plutonium (Pu-Tf), respectively, and one additional compartment describing plutonium in the interstitial fluids was performed successfully. The next step of the work is the modeling of the chelation process, coupling the physiologically modified structure with the biokinetic model for DTPA. RESULTS of animal studies performed under controlled conditions will enable to better understand the principles of the involved mechanisms.

  5. Uncertainty analysis of doses from ingestion of plutonium and americium.

    Science.gov (United States)

    Puncher, M; Harrison, J D

    2012-02-01

    Uncertainty analyses have been performed on the biokinetic model for americium currently used by the International Commission on Radiological Protection (ICRP), and the model for plutonium recently derived by Leggett, considering acute intakes by ingestion by adult members of the public. The analyses calculated distributions of doses per unit intake. Those parameters having the greatest impact on prospective doses were identified by sensitivity analysis; the most important were the fraction absorbed from the alimentary tract, f(1), and rates of uptake from blood to bone surfaces. Probability distributions were selected based on the observed distribution of plutonium and americium in human subjects where possible; the distributions for f(1) reflected uncertainty on the average value of this parameter for non-specified plutonium and americium compounds ingested by adult members of the public. The calculated distributions of effective doses for ingested (239)Pu and (241)Am were well described by log-normal distributions, with doses varying by around a factor of 3 above and below the central values; the distributions contain the current ICRP Publication 67 dose coefficients for ingestion of (239)Pu and (241)Am by adult members of the public. Uncertainty on f(1) values had the greatest impact on doses, particularly effective dose. It is concluded that: (1) more precise data on f(1) values would have a greater effect in reducing uncertainties on doses from ingested (239)Pu and (241)Am, than reducing uncertainty on other model parameter values and (2) the results support the dose coefficients (Sv Bq(-1) intake) derived by ICRP for ingestion of (239)Pu and (241)Am by adult members of the public.

  6. Properties of Liquid Plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Freibert, Franz J. [Los Alamos National Laboratory; Mitchell, Jeremy N. [Los Alamos National Laboratory; Schwartz, Daniel S. [Los Alamos National Laboratory; Saleh, Tarik A. [Los Alamos National Laboratory; Migliori, Albert [Los Alamos National Laboratory

    2012-08-02

    Unalloyed polycrystalline Pu displays extreme thermal expansion behavior, i.e., {alpha} {yields} {beta} {yields} {gamma} {yields} {delta} increases by 25% in volume and {delta} {yields} {var_epsilon} {yields} liquid decreases by 4.5% in volume. Thus, making it difficult to measure density into the liquid state. Dilatometer outfitted with CaF molten metal cell offers a proven capability to measure thermal expansion in molten metals, but has yet to be proven for Pu. Historic data from the liquid nuclear fuels program will prove extremely useful as a guide to future measurements. 3.3at% Ga changes Pu molten metal properties: 50% increase in viscosity and {approx}3% decrease in density. Fe may decrease the density by a small amount assuming an averaging of densities for Pu-Ga and Pu-Fe liquids. More recent Boivineau (2009) work needs some interpretation, but technique is being employed in (U,Pu)O{sub 2} nuclear fuels program (Pu Futures, 2012).

  7. The plutonium isotopic composition of marine biota on Enewetak Atoll: a preliminary assessment.

    Science.gov (United States)

    Hamilton, Terry F; Martinelli, Roger E; Kehl, Steven R; McAninch, Jeffrey E

    2008-10-01

    We have determined the level and distribution of gamma-emitting radionuclides, plutonium activity concentrations, and 240Pu/239Pu atom ratios in tissue samples of giant clam (Tridacna gigas and Hippopus hippopus), a top snail (Trochus nilaticas) and sea cucumber (Holothuria atra) collected from different locations around Enewetak Atoll. The plutonium isotopic measurements were performed using ultra-high sensitivity accelerator mass spectrometry (AMS). Elevated levels of plutonium were observed in the stomachs (includes the stomach lining) of Tridacna clam (0.62 to 2.98 Bq kg(-1), wet wt.), in the soft parts (edible portion) of top snails (0.25 to 1.7 Bq kg(-1)), wet wt.) and, to a lesser extent, in sea cucumber (0.015 to 0.22 Bq kg(-1), wet wt.) relative to muscle tissue concentrations in clam (0.006 to 0.021 Bq kg(-1), wet wt.) and in comparison with previous measurements of plutonium in fish. These data and information provide a basis for re-evaluating the relative significance of dietary intakes of plutonium from marine foods on Enewetak Atoll and, perhaps most importantly, demonstrate that discrete 240Pu239Pu isotope signatures might well provide a useful investigative tool to monitor source-term attribution and consequences on Enewetak Atoll. One potential application of immediate interest is to monitor and assess the health and ecological impacts of leakage of plutonium (as well as other radionuclides) from a low-level radioactive waste repository on Runit Island relative to background levels of fallout contamination in Enewetak Atoll lagoon.

  8. Recycle of scrap plutonium-238 oxide fuel to support future radioisotope applications

    Energy Technology Data Exchange (ETDEWEB)

    Schulte, L.D.; Espinoza, J.M.; Ramsey, K.B.; Rinehart, G.H.; Silver, G.L.; Purdy, G.M.; Jarvinen, G.D.

    1997-11-01

    The Nuclear Materials Technology (NMT) Division of Los Alamos National Laboratory has initiated a development program to recover and purify plutonium-238 oxide from impure feed sources in a glove box environment. A glove box line has been designed and a chemistry flowsheet developed to perform this recovery task at large scale. The initial demonstration effort focused on purification of {sup 238}PuO{sub 2} fuel by HNO{sub 3}/HF dissolution, followed by plutonium(III) oxalate precipitation and calcination to an oxide. Decontamination factors for most impurities of concern in the fuel were very good, producing {sup 238}PuO{sub 2} fuel significantly better in purity than specified by General Purpose Heat Source (GPHS) fuel powder specifications. The results are encouraging for recycle of relatively impure plutonium-238 oxide and scrap residue items into fuel for useful applications. A sufficient quantity of purified {sup 238}PuO{sub 2} fuel was recovered from the process to allow fabrication of a GPHS unit for testing. The high specific activity of plutonium-238 magnifies the consequences and concerns of radioactive waste generation. This work places an emphasis on development of waste minimization technologies to complement the aqueous processing operation. Results from experiments allowing more time for neutralized solutions of plutonium-238 to precipitate resulted in decontamination to about 1 millicurie/L. Combining ultrafiltration treatment with addition of a water-soluble polymer designed to coordinate Pu, allowed solutions to be decontaminated to about 1 microcurie/L. Efforts continue to develop a capability for efficient, safe, cost-effective, and environmentally acceptable methods to recover and purify {sup 238}PuO{sub 2} fuel.

  9. Plutonium distribution and remobilization in sediments of the Rhone River mouth (North-Western Mediterranean); Distribution et remobilisation du plutonium dans les sediments du prodelta du Rhone (Mediterranee nord-occidentale)

    Energy Technology Data Exchange (ETDEWEB)

    Lansard, B

    2004-06-15

    The aim of the present study was to describe the distribution and remobilization of plutonium (Pu) in the sediments off the Rhone river mouth. Most of the {sup 238}Pu and {sup 239,240}Pu isotopes introduced into the Rhone River were discharged by the liquid effluents released from the Marcoule reprocessing plant, located 120 km upstream the river mouth. Due to its high affinity for particles and its long half life, {sup 238}Pu is a promising tracer to follow the dispersion of particulate matter from the Rhone River to the Mediterranean Sea. During the 3 REMORA cruises, sediment samples were specifically collected in the Rhone pro-delta area and more offshore on the whole continental shelf of the Gulf of Lions. The measurements of alpha emitters gave a first detailed spatial distribution of Pu isotope concentrations in surface sediments off the Rhone mouth. Using {sup 137}Cs concentrations and their correlations with Pu isotopes, we were able to give a first estimate of Pu inventories for the sediments of the study area. In 2001, plutonium inventories were estimated to 92 {+-} 7 GBq of {sup 238}Pu and 522 {+-} 44 GBq of {sup 239,240}Pu for an area of 500 km{sup 2} in front of the Rhone River mouth. Roughly, 50 % of these inventories are trapped in an area of 100 km{sup 2} corresponding to the extent of the Rhone pro-delta zone. In spring 2002, an ADCP, with current velocity and wave measurements, was moored off the Rhone River mouth. This unique in situ dataset highlights the major role of South-East swells in the erosion of pro-deltaic sediments and their dispersion to the South-Westward direction. Plutonium remobilization was examined using a new experimental design based on sediment resuspension processes studied within a linear recirculating flume. For Gulf of Lions sediments and for a given hydrodynamic stress, remobilization fluxes raised a maximum of 0.08 Bq.m{sup -2}.h{sup -1} for {sup 238}Pu and 0.64 Bq.m{sup -2}.h{sup -1} for {sup 239,240}Pu. A first

  10. FEASIBILITY OF RECYCLING PLUTONIUM AND MINOR ACTINIDES IN LIGHT WATER REACTORS USING HYDRIDE FUEL

    Energy Technology Data Exchange (ETDEWEB)

    Greenspan, Ehud; Todreas, Neil; Taiwo, Temitope

    2009-03-10

    The objective of this DOE NERI program sponsored project was to assess the feasibility of improving the plutonium (Pu) and minor actinide (MA) recycling capabilities of pressurized water reactors (PWRs) by using hydride instead of oxide fuels. There are four general parts to this assessment: 1) Identifying promising hydride fuel assembly designs for recycling Pu and MAs in PWRs 2) Performing a comprehensive systems analysis that compares the fuel cycle characteristics of Pu and MA recycling in PWRs using the promising hydride fuel assembly designs identified in Part 1 versus using oxide fuel assembly designs 3) Conducting a safety analysis to assess the likelihood of licensing hydride fuel assembly designs 4) Assessing the compatibility of hydride fuel with cladding materials and water under typical PWR operating conditions Hydride fuel was found to offer promising transmutation characteristics and is recommended for further examination as a possible preferred option for recycling plutonium in PWRs.

  11. Oxidation-state distribution of plutonium in surface and subsurface waters at Thule, northwest Greenland

    DEFF Research Database (Denmark)

    McMahon, C.A.; Vintró, L.L.; Mitchell, P.I.

    2000-01-01

    chemical form) is present as fully dissolved species. Most of this plutonium would seem to be of weapons fallout origin, as the mean Pu-238/Pu-239,Pu-240 activity ratio in the water column (dissolved phase) at Thule (0.06 +/- 0.02; n = 10) is similar to the global fallout ratio at this latitude......The speciation of plutonium in Arctic waters sampled on the northwest Greenland shelf in August 1997 is discussed in this paper. Specifically, we report the results of analyses carried out on seawater sampled (a) close to the Thule air base where, in 1968, a US military aircraft carrying four......(V, VI) (mean, 68 +/- 6%; n = 6), with little if any distinction apparent between surface and bottom waters. Further, the oxidation state distribution at stations close to the accident site is similar to that measured at Upernavik, remote from this site. It is also similar to the distribution observed...

  12. (137)Cs, (239+240)Pu concentrations and the (240)Pu/(239)Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary.

    Science.gov (United States)

    Pan, S M; Tims, S G; Liu, X Y; Fifield, L K

    2011-10-01

    A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of (137)Cs and plutonium (Pu) isotopes. The (137)Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the (137)Cs and (239+240)Pu. The shape of the vertical (137)Cs distribution in the sediment core was similar to that of the Pu. The maximum (137)Cs and (239+240)Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average (240)Pu/(239)Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the (240)Pu/(239)Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The (137)Cs and (239+240)Pu inventories were estimated to be 7100 ± 1200 Bq/m(2) and 407 ± 27 Bq/m(2), respectively. Approximately 40% of the (239+240)Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure (240)Pu/(239)Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.

  13. Chemical separation and ICP-AES determination of 22 metallic elements in U and Pu matrices using cyanex-923 extractant and studies on stripping of U and Pu.

    Science.gov (United States)

    Argekar, A A; Kulkarni, M J; Mathur, J N; Page, A G

    2002-03-11

    Comprehensive studies have been carried out on the extraction behavior of uranium and plutonium matrices using cyanex-923 extractant. The near total extraction of U/Pu and quantitative separation of 22 metallic elements at trace levels has been established using inductively coupled plasma-atomic emission spectrometry (ICP-AES). The studies carried out on back extraction of U/Pu from organic phase have established the near total recovery of these matrices into the aqueous phase using 1 M Na(2)CO(3) and saturated oxalic acid, respectively.

  14. Research Program to Determine Redox Reactions and Their Effects on Speciation and Mobility of Plutonium in DOE Wastes

    Energy Technology Data Exchange (ETDEWEB)

    Choppin, G.R.; Rai, D.

    2000-10-01

    Plutonium in geologic matrices undergoes a variety of complex reactions which complicate its environmental behavior. These complexities in plutonium chemistry whereby a large variety of precipitation, dissolution, adsorption/desorption, and redox reactions control plutonium speciation and concentrations, result in the need for a rather large amount of reliable, fundamental data to predict Pu behavior in geologic media. These data are also needed for evaluation of remediation strategies that involve removing most of the contaminants by selective methods, followed by in situ immobilization of residual contaminants. Two areas were studied during this project: (1) thermodynamic data for Th(IV) and Pu(IV) complexes of EDTA and for Pu(V) interactions with chloride; (2) kinetic data for redox reactions of Pu in the presence of common redox agents (e.g., H{sub 2}O{sub 2}, MnO{sub 2}, and NaOCl) encountered under waste disposal conditions. These studies are relevant to understanding Pu behavior in wastes disposed of in diverse geologic conditions (e.g., at the WIPP and YUCCA Mountain repositories and in contaminated sediments at many different DOE sites) and also for developing effective remediation strategies (e.g., processing of high level waste tanks). These studies have yielded data to address redox reactions of plutonium in the presence of environmentally important agents (e.g. organic and inorganic oxidants/reductants).

  15. On problem of ultrasensitive determination of man-made plutonium in living species

    CERN Document Server

    Perelygin, V P; Dmitriev, S N; Oganessian, Yu T; Petrova, R I; Drobina, T P

    1999-01-01

    To improve the sensitivity of the method of Pu determination in specimens we applied two additional steps of chemical separation of Pu from U. After the usual chemical separation of Pu we used second step with ion-exchange column, where the ions of U sup 4 sup + were absorbed by sorbent and Pu sup 3 sup + ions remains in solution. For converting Plutonium to Pu sup 3 sup + state the electrochemical procedure has been used. After the electrochemical separation procedure the solution was deposited onto quartz glass. Then the quartz glass plates were inserted into the gas mixture flow (SOCL sub 2 +air) at the temperature 650 deg. C. Such a procedure extracts >=90% U from Pu layer. Now we provide the chemical separation of Pu from U by a factor >=10 sup 7. It means that now we are able to perform the routine Pu analysis at the level of sensitivity 10 sup - sup 1 sup 4 -10 sup - sup 1 sup 5 g/g. By using combined n-gamma activation technique we can determine the Pu content in the small fragments of tissues of livi...

  16. Plutonium(IV) sorption to montmorillonite in the presence of organic matter.

    Science.gov (United States)

    Boggs, Mark A; Dai, Zurong; Kersting, Annie B; Zavarin, Mavrik

    2015-03-01

    The effect of altering the order of addition in a ternary system of plutonium(IV), organic matter (fulvic acid, humic acid and desferrioxamine B), and montmorillonite was investigated. A decrease in Pu(IV) sorption to montmorillonite in the presence of fulvic and humic acid relative to the binary Pu-montmorillonite system, is attributed to strong organic aqueous complex formation with aqueous Pu(IV). No dependence on the order of addition was observed. In contrast, in the system where Pu(IV) was equilibrated with desferrioxamine B (DFOB) prior to addition of montmorillonite, an increase in Pu(IV) sorption was observed relative to the binary system. When DFOB was equilibrated with montmorillonite prior to addition of Pu(IV), Pu(IV) sorption was equivalent to the binary system. X-ray diffraction and transmission electron microscopy revealed that DFOB accumulated in the interlayer of montmorillonite. The order of DFOB addition plays an important role in the observed sorption/desorption behavior of Pu. The irreversible nature of DFOB accumulation in the montmorillonite interlayer leads to an apparent dependence of Pu sorption on the order of addition in the ternary system. This work demonstrates that the order of addition will be relevant in ternary systems in which at least one component exhibits irreversible sorption behavior.

  17. Plutonium isotopes and 241Am in the atmosphere of Lithuania: A comparison of different source terms

    Science.gov (United States)

    Lujanienė, G.; Valiulis, D.; Byčenkienė, S.; Šakalys, J.; Povinec, P. P.

    2012-12-01

    137Cs, 241Am and Pu isotopes collected in aerosol samples during 1994-2011 were analyzed with special emphasis on better understanding of Pu and Am behavior in the atmosphere. The results from long-term measurements of 240Pu/239Pu atom ratios showed a bimodal frequency distribution with median values of 0.195 and 0.253, indicating two main sources contributing to the Pu activities at the Vilnius sampling station. The low Pu atom ratio of 0.141 could be attributed to the weapon-grade plutonium derived from the nuclear weapon test sites. The frequency of air masses arriving from the North-West and North-East correlated with the Pu atom ratio indicating the input from the sources located in these regions (the Novaya Zemlya test site, Siberian nuclear plants), while no correlation with the Chernobyl region was observed. Measurements carried out during the Fukushima accident showed a negligible impact of this source with Pu activities by four orders of magnitude lower as compared to the Chernobyl accident. The activity concentration of actinides measured in the integrated sample collected in March-April, 2011 showed a small contribution of Pu with unusual activity and atom ratios indicating the presence of the spent fuel of different origin than that of the Chernobyl accident.

  18. Plutonium(IV) precipitates formed in alkaline media in the presence of various anions

    Energy Technology Data Exchange (ETDEWEB)

    Krot, N.N.; Shilov, V.P.; Yusov, A.B.; Tananaev, I.G.; Grigoriev, M.S.; Garnov, A.Yu.; Perminov, V.P.; Astafurova, L.N.

    1998-09-01

    The tendency of Pu(IV) to hydrolyze and form true solutions, colloid solutions, or insoluble precipitates has been known since the Manhattan Project. Since then, specific studies have been performed to examine in detail the equilibria of Pu(IV) hydrolytic reactions in various media. Great attention also has been paid to the preparation, structure, and properties of Pu(IV) polymers or colloids. These compounds found an important application in sol-gel technology for the preparation of nuclear fuel materials. A most important result of these works was the conclusion that Pu(IV) hydroxide, after some aging, consists of very small PuO{sub 2} crystallites and should therefore be considered to be Pu(IV) hydrous oxide. However, studies of the properties and behavior of solid Pu(IV) hydroxide in complex heterogeneous systems are rare. The primary goal of this investigation was to obtain data on the composition and properties of Pu(IV) hydrous oxide or other compounds formed in alkaline media under different conditions. Such information is important to understand Pu(IV) behavior and the forms of its existence in the Hanford Site alkaline tank waste sludge. This knowledge then may be applied in assessing plutonium criticality hazards in the storage, retrieval, and treatment of Hanford Site tank wastes as well as in understanding its contribution to the transuranic waste inventory (threshold at 100 nCi/g or about 5 {times} 10{sup {minus}6} M) of the separate solution and solid phases.

  19. Investigation of Pu (Ⅳ) toxicity by computer simulation in human body fliuds%计算机模拟研究钚(Ⅳ)的人体毒性

    Institute of Scientific and Technical Information of China (English)

    邓冰; 王和义; 蒋树斌

    2013-01-01

    引入Ca2+、Fe3+、Zn2+、Mn2+等金属离子和氨基酸、柠檬酸、乳酸等小分子配体建立了Pu4+在人体血浆、胃液、组织液、细胞液等主要体液中的金属离子-小分子配体热力学平衡模型.利用该模型研究了正常生理条件下Pu(Ⅳ)在各体液中的存在形态以及pH值和[Pu]改变对Pu(Ⅳ)形态的影响.结果表明,血浆中的低浓度Pu(Ⅳ)易以Pu(OH)4 (aq)的形态蓄积在肝脏中,钚浓度升高则形成沉淀难以排出;胃液中的Pu(Ⅳ)可大量进入血液中,但胃液pH值升高可实现钚的促排;组织液中钚会沉积在骨骼无机表面;高浓度Pu(Ⅳ)对大多数细胞有极高毒性;随着尿液的pH值增大,沉积的Pu(OH)4(s)会对肾脏造成损伤;胰液中的Pu(Ⅳ)的形态随着pH值改变而发生显著变化,而胆汁中高钚含量的Pu(Ⅳ)易滞留在肝脏内;在正常汗液pH值波动范围内,Pu(Ⅳ)易进入人体,从而对钚操作人员的健康产生危害.%A thermodynamic equilibrium model, involved in major metal-ions and low molecular weight molecule ligands, was developed to analyze the speciation of Pu4+ in human body fluids, including plasma fluid, gastric juice, human intracellular, and interstitial etc. Under the normal physiological condition, the model was used to research the influence of the change of pH value and the concentration of plutonium on the speciation of Pu( Ⅳ) in various body fluids. The results indicated that low concentration of plutonium in plasma fluid as Pu(OH)4(aq) species was accumulated in liver. Pu4+ formed precipitation and was difficult to eliminate from the body under the high concentration of plutonium in plasma fluid. Through the gastric juice Pu4 + can enter the blood stream. Increasing pH value of gastric juice can promote the excretion of plutonium. Pu(Ⅳ) deposited on the bone mineral surface in the interstitial and high concentration of Pu( Ⅳ) was extremely toxic for most cells. With the increase of p

  20. Polonium, uranium and plutonium radionuclides in aquatic and land ecosystem of Poland.

    Science.gov (United States)

    Skwarzec, Bogdan; Strumińska-Parulska, Dagmara I; Boryło, Alicja; Kabat, Krzysztof

    2012-01-01

    This article presents the results of study about distribution, inflow and accumulation of polonium, uranium and plutonium in aquatic and land environment of Poland and the southern Baltic Sea. Radionuclides of (210)Po, (234)U and (238)U as well as (239+240)Pu and (241)Pu are strongly accumulated in Baltic organisms and plants and transferred through the trophic chain. The values of bioconcentration factor (BCF) in Baltic plants and animals are higher for polonium and plutonium in comparison with uranium. The principal source of radionuclides in the southern Baltic Sea is their inflow with rivers. Total annual runoff of polonium, uranium and plutonium from the Vistula and the Odra as well as the Pomeranian rivers were calculated at 95 GBq of (210)Po, 750 GBq of (234+238)U and 160 MBq of (238+239+240)Pu. Seasonal and spatial variability of (210)Po, (238)U and (239+240)Pu levels in the Vistula and the Odra drainage basins were assessed by application of neural-network based classification, especially cluster analysis (CA), principal component analysis (PCA) and self-organizing maps (SOM). The result for the Vistula river indicated correlation between polonium and plutonium as well as polonium and uranium. In the Odra drainage basin, the biggest differences were observed in the case of (238)U. To assess if there are statistically significant differences in mean concentration values of (210)Po, (238)U and (239+240)Pu for the Vistula and the Odra rivers drainage basins were obtained by used of the non-parametric tests. Comparing to the Vistula catchment area, statistically differences concentration of (210)Po and (239+240)Pu in all year was observed for river samples collected on the Odra drainage basin.

  1. {sup 241}Pu concentrations in water, plankton and fish from the southern Baltic Sea

    Energy Technology Data Exchange (ETDEWEB)

    Struminska-Parulska, D.I.; Skwarzec, B. [Gdansk, Univ. (Poland). Facuty of Chemistry

    2013-08-01

    The aim of the work was to determine {sup 241}Pu activities in different components (water, plankton and fish) of the southern Baltic Sea ecosystem. Measurement of {sup 241}Pu in the samples was done indirectly by determining the increment in {sup 241}Am from the decay of the {beta}-emitting {sup 241}Pu in samples collected 10-15 years after the Chernobyl accident. Enhanced levels of {sup 241}Pu were observed in all analyzed Baltic samples. The highest {sup 241}Pu concentrations in fish were found in Perciformes: benthic round goby (0.863 {+-} 0.066 mBq/g ww) and pelagic perch (0.666 {+-} 0.001 mBq/g ww). Plutonium is also non-uniformly distributed in the organs and tissues of the analyzed fish; especially pelagic herring and cod as well as benthic flounder. Most of {sup 241}Pu in flounder, herring and cod is located in soft tissues, especially digestive organs (stomach, intestine, liver). The annual individual effective doses calculated on the basis of {sup 241}Pu concentrations in fish indicated that the impact of the consumption of {sup 241}Pu containing Baltic fish on the annual effective dose for a statistical inhabitant of Poland was very small. (orig.)

  2. Capability to Recover Plutonium-238 in H-Canyon/HB-Line - 13248

    Energy Technology Data Exchange (ETDEWEB)

    Fuller, Kenneth S. Jr.; Smith, Robert H. Jr.; Goergen, Charles R. [Savannah River Nuclear Solutions, LLC, Savannah River Site, Aiken, SC 29802 (United States)

    2013-07-01

    Plutonium-238 is used in Radioisotope Thermoelectric Generators (RTGs) to generate electrical power and in Radioisotope Heater Units (RHUs) to produce heat for electronics and environmental control for deep space missions. The domestic supply of Pu-238 consists of scrap material from previous mission production or material purchased from Russia. Currently, the United States has no significant production scale operational capability to produce and separate new Pu-238 from irradiated neptunium-237 targets. The Department of Energy - Nuclear Energy is currently evaluating and developing plans to reconstitute the United States capability to produce Pu-238 from irradiated Np-237 targets. The Savannah River Site had previously produced and/or processed all the Pu-238 utilized in Radioisotope Thermoelectric Generators (RTGs) for deep space missions up to and including the majority of the plutonium for the Cassini Mission. The previous full production cycle capabilities included: Np- 237 target fabrication, target irradiation, target dissolution and Np-237 and Pu-238 separation and purification, conversion of Np-237 and Pu-238 to oxide, scrap recovery, and Pu-238 encapsulation. The capability and equipment still exist and could be revitalized or put back into service to recover and purify Pu-238/Np-237 or broken General Purpose Heat Source (GPHS) pellets utilizing existing process equipment in HB-Line Scrap Recovery, and H-Canyon Frame Waste Recovery processes. The conversion of Np-237 and Pu-238 to oxide can be performed in the existing HB-Line Phase-2 and Phase- 3 Processes. Dissolution of irradiated Np-237 target material, and separation and purification of Np-237 and Pu-238 product streams would be possible at production rates of ∼2 kg/month of Pu-238 if the existing H-Canyon Frames Process spare equipment were re-installed. Previously, the primary H-Canyon Frames equipment was removed to be replaced: however, the replacement project was stopped. The spare equipment

  3. CAPABILITY TO RECOVER PLUTONIUM-238 IN H-CANYON/HB-LINE

    Energy Technology Data Exchange (ETDEWEB)

    Fuller, Kenneth S. Jr.; Smith, Robert H. Jr.; Goergen, Charles R.

    2013-01-09

    Plutonium-238 is used in Radioisotope Thermoelectric Generators (RTGs) to generate electrical power and in Radioisotope Heater Units (RHUs) to produce heat for electronics and environmental control for deep space missions. The domestic supply of Pu-238 consists of scrap material from previous mission production or material purchased from Russia. Currently, the United States has no significant production scale operational capability to produce and separate new Pu-238 from irradiated neptunium-237 targets. The Department of Energy - Nuclear Energy is currently evaluating and developing plans to reconstitute the United States capability to produce Pu-238 from irradiated Np-237 targets. The Savannah River Site had previously produced and/or processed all the Pu-238 utilized in Radioisotope Thermoelectric Generators (RTGs) for deep space missions up to and including the majority of the plutonium for the Cassini Mission. The previous full production cycle capabilities included: Np-237 target fabrication, target irradiation, target dissolution and Np-237 and Pu-238 separation and purification, conversion of Np-237 and Pu-238 to oxide, scrap recovery, and Pu-238 encapsulation. The capability and equipment still exist and could be revitalized or put back into service to recover and purify Pu-238/Np-237 or broken General Purpose Heat Source (GPHS) pellets utilizing existing process equipment in HB-Line Scrap Recovery, and H-anyon Frame Waste Recovery processes. The conversion of Np-237 and Pu-238 to oxide can be performed in the existing HB-Line Phase-2 and Phase-3 Processes. Dissolution of irradiated Np-237 target material, and separation and purification of Np-237 and Pu-238 product streams would be possible at production rates of ~ 2 kg/month of Pu-238 if the existing H-Canyon Frames Process spare equipment were re-installed. Previously, the primary H-Canyon Frames equipment was removed to be replaced: however, the replacement project was stopped. The spare equipment is

  4. Formation of Pu(III) colloids observed by laser-induced breakdown detection

    Energy Technology Data Exchange (ETDEWEB)

    Cho, H. R.; Cha, W.; Park, K. K.; Jung, E. C. [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

    2015-05-15

    In the present work, the reduction conditions were controlled through electrolysis. An electrochemical cell with a Teflon vessel and quartz tubes containing electrodes were installed in a glove-box purged with Ar gas to prepare plutonium samples at different pHs under reducing condition. The concentration of hydrogen ions (H{sup +}) of plutonium solutions was reduced using an electric current from a Ag/AgCl reference electrode to a Pt working electrode, which called coulometric pH titration. The electrolytic reducing condition maintains the dominant oxidation state of Pu(III). Soluble species were investigated using absorption spectroscopy adopting a liquid waveguide capillary cell (LWCC) which has an optical path length of 100 cm. The formation of plutonium hydroxide colloids and solubility were determined by laser-induced breakdown detection (LIBD). Electrolytic reduction was a useful method to investigate the hydrolysis, colloid formation and solubility of Pu(III) hydroxide. The oxidation state of Pu(III) maintained well during the reduction of hydrogen ions being comparable to strong reducing agents such as Fe powder. The determined solubility product was lower than the reported data by Felmy et al. . The existence of Pu(IV), which can result in lower solubility investigated by measurement of redox potentials of samples will be presented in detail.

  5. METHOD OF PRODUCING PLUTONIUM TETRAFLUORIDE

    Science.gov (United States)

    Tolley, W.B.; Smith, R.C.

    1959-12-15

    A process is presented for preparing plutonium tetrafluoride from plutonium(IV) oxalate. The oxalate is dried and decomposed at about 300 deg C to the dioxide, mixed with ammonium bifluoride, and the mixture is heated to between 50 and 150 deg C whereby ammonium plutonium fluoride is formed. The ammonium plutonium fluoride is then heated to about 300 deg C for volatilization of ammonium fluoride. Both heating steps are preferably carried out in an inert atmosphere.

  6. Plutonium dissolution process

    Science.gov (United States)

    Vest, M.A.; Fink, S.D.; Karraker, D.G.; Moore, E.N.; Holcomb, H.P.

    1994-01-01

    A two-step process for dissolving Pu metal is disclosed in which two steps can be carried out sequentially or simultaneously. Pu metal is exposed to a first mixture of 1.0-1.67 M sulfamic acid and 0.0025-0.1 M fluoride, the mixture having been heated to 45-70 C. The mixture will dissolve a first portion of the Pu metal but leave a portion of the Pu in an oxide residue. Then, a mineral acid and additional fluoride are added to dissolve the residue. Alternatively, nitric acid between 0.05 and 0.067 M is added to the first mixture to dissolve the residue as it is produced. Hydrogen released during the dissolution is diluted with nitrogen.

  7. First-principles elastic properties of (alpha)-Pu

    Energy Technology Data Exchange (ETDEWEB)

    Soderlind, P; Klepeis, J E

    2008-11-04

    Density-functional electronic structure calculations have been used to investigate the ambient pressure and low temperature elastic properties of the ground-state {alpha} phase of plutonium metal. The electronic structure and correlation effects are modeled within a fully relativistic anti-ferromagnetic treatment with a generalized gradient approximation for the electron exchange and correlation functionals. The 13 independent elastic constants, for the monoclinic {alpha}-Pu system, are calculated for the observed geometry. A comparison of the results with measured data from resonant ultrasound spectroscopy for a cast sample is made.

  8. First-principles elastic properties of (alpha)-Pu

    Energy Technology Data Exchange (ETDEWEB)

    Soderlind, P; Klepeis, J

    2009-02-18

    Density-functional electronic-structure calculations have been used to investigate the ambient pressure and low temperature elastic properties of the ground-state {alpha} phase of plutonium metal. The electronic structure and correlation effects are modeled within a fully relativistic antiferromagnetic treatment with a generalized gradient approximation for the electron exchange and correlation functional. The 13 independent elastic constants, for the monoclinic {alpha}-Pu system, are calculated for the observed geometry. A comparison of the results with measured data from recent resonant ultrasound spectroscopy for a cast sample is made.

  9. Status of plutonium ceramic immobilization processes and immobilization forms

    Energy Technology Data Exchange (ETDEWEB)

    Ebbinghaus, B.B.; Van Konynenburg, R.A. [Lawrence Livermore National Lab., CA (United States); Vance, E.R.; Jostsons, A. [Australian Nuclear Science and Technology Organization, Menai (Australia)] [and others

    1996-05-01

    Immobilization in a ceramic followed by permanent emplacement in a repository or borehole is one of the alternatives currently being considered by the Fissile Materials Disposition Program for the ultimate disposal of excess weapons-grade plutonium. To make Pu recovery more difficult, radioactive cesium may also be incorporated into the immobilization form. Valuable data are already available for ceramics form R&D efforts to immobilize high-level and mixed wastes. Ceramics have a high capacity for actinides, cesium, and some neutron absorbers. A unique characteristic of ceramics is the existence of mineral analogues found in nature that have demonstrated actinide immobilization over geologic time periods. The ceramic form currently being considered for plutonium disposition is a synthetic rock (SYNROC) material composed primarily of zirconolite (CaZrTi{sub 2}O{sub 7}), the desired actinide host phase, with lesser amounts of hollandite (BaAl{sub 2}Ti{sub 6}O{sub 16}) and rutile (TiO{sub 2}). Alternative actinide host phases are also being considered. These include pyrochlore (Gd{sub 2}Ti{sub 2}O{sub 7}), zircon (ZrSiO{sub 4}), and monazite (CePO{sub 4}), to name a few of the most promising. R&D activities to address important technical issues are discussed. Primarily these include moderate scale hot press fabrications with plutonium, direct loading of PuO{sub 2} powder, cold press and sinter fabrication methods, and immobilization form formulation issues.

  10. AFS-2 FLOWSHEET MODIFICATIONS TO ADDRESS THE INGROWTH OF PU(VI) DURING METAL DISSOLUTION

    Energy Technology Data Exchange (ETDEWEB)

    Crapse, K.; Rudisill, T.; O' Rourke, P.; Kyser, E.

    2014-07-02

    In support of the Alternate Feed Stock Two (AFS-2) PuO{sub 2} production campaign, Savannah River National Laboratory (SRNL) conducted a series of experiments concluding that dissolving Pu metal at 95°C using a 6–10 M HNO{sub 3} solution containing 0.05–0.2 M KF and 0–2 g/L B could reduce the oxidation of Pu(IV) to Pu(VI) as compared to dissolving Pu metal under the same conditions but at or near the boiling temperature. This flowsheet was demonstrated by conducting Pu metal dissolutions at 95°C to ensure that PuO{sub 2} solids were not formed during the dissolution. These dissolution parameters can be used for dissolving both Aqueous Polishing (AP) and MOX Process (MP) specification materials. Preceding the studies reported herein, two batches of Pu metal were dissolved in the H-Canyon 6.1D dissolver to prepare feed solution for the AFS-2 PuO{sub 2} production campaign. While in storage, UV-visible spectra obtained from an at-line spectrophotometer indicated the presence of Pu(VI). Analysis of the solutions also showed the presence of Fe, Ni, and Cr. Oxidation of Pu(IV) produced during metal dissolution to Pu(VI) is a concern for anion exchange purification. Anion exchange requires Pu in the +4 oxidation state for formation of the anionic plutonium(IV) hexanitrato complex which absorbs onto the resin. The presence of Pu(VI) in the anion feed solution would require a valence adjustment step to prevent losses. In addition, the presence of Cr(VI) would result in absorption of chromate ion onto the resin and could limit the purification of Pu from Cr which may challenge the purity specification of the final PuO{sub 2} product. Initial experiments were performed to quantify the rate of oxidation of Pu(IV) to Pu(VI) (presumed to be facilitated by Cr(VI)) as functions of the HNO{sub 3} concentration and temperature in simulated dissolution solutions containing Cr, Fe, and Ni. In these simulated Pu dissolutions studies, lowering the temperature from near boiling

  11. Preparation of a multi-isotope plutonium AMS standard and preliminary results of a first inter-lab comparison

    Science.gov (United States)

    Dittmann, B.-A.; Dunai, T. J.; Dewald, A.; Heinze, S.; Feuerstein, C.; Strub, E.; Fifield, L. K.; Froehlich, M. B.; Tims, S. G.; Wallner, A.; Christl, M.

    2015-10-01

    The motivation of this work is to establish a new multi-isotope plutonium standard for isotopic ratio measurements with accelerator mass spectrometry (AMS), since stocks of existing solutions are declining. To this end, certified reference materials (CRMs) of each of the individual isotopes 239Pu, 240Pu, 242Pu and 244Pu were obtained from JRC IRMM (Joint Research Center Institute for Reference Materials and Measurements). These certified reference materials (IRMM-081a, IRMM-083, IRMM-043 and IRMM-042a) were diluted with nitric acid and mixed to obtain a stock standard solution with an isotopic ratio of approximately 1.0:1.0:1.0:0.1 (239Pu:240Pu:242Pu:244Pu). From this stock solution, samples were prepared for measurement of the plutonium isotopic composition by AMS. These samples have been measured in a round-robin exercise between the AMS facilities at CologneAMS, at the ANU Canberra and ETH Zurich to verify the isotopic ratio and to demonstrate the reproducibility of the measurements. The results show good agreement both between the different AMS measurements and with the gravimetrically determined nominal ratios.

  12. Preparation of reference material for uranium and plutonium measurements using cellulose compound as a stabilizer

    Energy Technology Data Exchange (ETDEWEB)

    Surugaya, Naoki; Sato, Soichi; Hina, Tetsuro; Hiyama, Toshiaki [Japan Nuclear Cycle Development Inst., Tokai Works, Tokai, Ibaraki (Japan)

    2003-03-01

    Isotope dilution mass spectrometry, considered the most reliable analytical technique for input accountancy measurements of uranium and plutonium in spent fuel reprocessing plants, requires a well-characterized uranium/plutonium spike. Solid spikes containing {sup 235}U and {sup 239}Pu have been successfully utilized in safeguards inspections and in accountability analysis. They contain relatively large amounts of uranium and plutonium isotopically different to the uranium and plutonium of the sample, and are usually in the dried nitrate form. However, it is difficult to maintain and guarantee the integrity of the spike over long periods as they are in the dried nitrate form that can flake off the glass ampoule surface. Organic coatings were investigated using cellulose acetate butyrate as a stabilizer. The cellulose acetate butyrate had good characteristics, maintaining a thin film for a long time. (author)

  13. Sonochemical Digestion of High-Fired Plutonium Dioxide Samples

    Energy Technology Data Exchange (ETDEWEB)

    Sinkov, Sergei I.; Lumetta, Gregg J.

    2006-10-12

    of PuO2 can be achieved with 6 to 8 M nitric acid + 14 M HF or 8 M nitric acid + 4 M HF mixtures. In the latter case, quantitative dissolution of plutonium oxide was demonstrated only with sonication. Overall, the results indicate that applying ultrasound in an isolated cup horn configuration to dissolve refractory plutonium oxide does not offer any substantial advantage over conventional ?heat and mix? treatment. Oxidative treatment by AgO appears to be effective only when very little or no oxidizable materials are present in the digested sample. The catalytic use of Ag(II) in the ''Catalyzed Electrolytic Plutonium Oxide Dissolution'' technology would probably be more effective than using AgO because the Ag(II) is continually regenerated electrochemically. Reductive treatment with titanium trichloride in HCl solution proves to be less efficient than the previously observed effect based on in situ generation of Ti(III) in phosphoric acid and sulfuric acid media using a dip probe sonication setup. The previous experiments, however, were performed at higher temperature and with non-steady concentration profiles of Ti(III) ion in the process of sonochemical digestion.

  14. Desorption of plutonium from montmorillonite: An experimental and modeling study

    Science.gov (United States)

    Begg, James D.; Zavarin, Mavrik; Kersting, Annie B.

    2017-01-01

    Desorption of plutonium (Pu) will likely control the extent to which it is transported by mineral colloids. We evaluated the adsorption/desorption behavior of Pu on SWy-1 montmorillonite colloids at pH 4, pH 6, and pH 8 using batch adsorption and flow cell desorption experiments. After 21 days adsorption, Pu(IV) affinity for montmorillonite displayed a pH dependency, with Kd values highest at pH 4 and lowest at pH 8. The pH 8 experiment was further allowed to equilibrate for 6 months and showed an increase in Kd, indicating that true sorption equilibrium was not achieved within the first 21 days. For the desorption experiments, aliquots of the sorption suspensions were placed in a flow cell, and Pu-free solutions were then pumped through the cell for a period of 12 days. Changes in influent solution flow rate were used to investigate the kinetics of Pu desorption and demonstrated that it was rate-limited over the experimental timescales. At the end of the 12-day flow cell experiments, the extent of desorption was again pH dependent, with pH 8 > pH 6 > pH 4. Further, at pH 8, less Pu was desorbed after an adsorption contact time of 6 months than after a contact time of 21 days, consistent with an aging of Pu on the clay surface. A conceptual model for Pu adsorption/desorption that incorporated known surface-mediated Pu redox reactions was used to fit the experimental data. The resulting rate constants indicated processes occurring on timescales of months and even years which may, in part, explain observations of clay colloid-facilitated Pu transport on decadal timescales. Importantly, however, our results also imply that migration of Pu adsorbed to montmorillonite colloids at long (50-100 year) timescales under oxic conditions may not be possible without considering additional phenomena, such as co-precipitation.

  15. Economical Production of Pu-238: NIAC Phase I Final Report

    Science.gov (United States)

    Howe, Steven D.; Crawford, Douglas; Navarro, Jorge; O'Brien, Robert C.; Katalenich, Jeff; Ring, Terry

    2016-01-01

    All space exploration missions traveling beyond Jupiter must use radioisotopic power sources for electrical power. The best isotope to power these sources is plutonium-238 (Pu-238). The US supply of Pu-238 is almost exhausted and will be gone within the next decade. The Department of Energy has initiated a production program with a $10M allocation from NASA but the cost is estimated at over $100M to get to production levels. The Center for Space Nuclear Research (CSNR) has conceived of a potentially better process to produce Pu-238 earlier and for significantly less cost. Potentially, the front end capital costs could be provided by private industry such that the government only had to pay for the product produced. In the Phase I NIAC (NASA Innovative Advanced Concepts) grant, the CSNR has evaluated the feasibility of using a low power, commercially available nuclear reactor to produce 1.5 kg of Pu-238 per year. The impact on the neutronics of the reactor have been assessed, the amount of Neptunium target material estimated, and the production rates calculated. In addition, the size of the post-irradiation processing facility has been established. Finally, as the study progressed, a new method for fabricating the Pu-238 product into the form used for power sources has been identified to reduce the cost of the final product. In short, the concept appears to be viable, can produce the amount of Pu-238 needed to support the NASA missions, can be available within a few years, and will cost significantly less than the current DOE program.

  16. Selection and Evaluation of a new Pu Density Measurement Fluid

    Energy Technology Data Exchange (ETDEWEB)

    Dziewinska, Krystyna [Los Alamos National Laboratory; Peters, Michael A [Los Alamos National Laboratory; Martinez, Patrick P [Los Alamos National Laboratory; Dziewinski, Jacek J [Los Alamos National Laboratory; Pugmire, David L [Los Alamos National Laboratory; Trujillo, Stephen M [Los Alamos National Laboratory; La Verne, Jake A [UNIV OF NOTRE DAME; Rajesh, P [UNIV OF NOTRE DAME

    2009-01-01

    This paper summarizes efforts leading to selection of a new fluid for the determination of the density of large Pu parts. Based on an extended literature search, perfluorotributylamine (FC-43) was chosen for an experimental study. Plutonium coupon corrosion studies were performed by exposing Pu to deaerated and aerated solutions and measuring corrosion gravimetrically. Corrosion rates were determined. Samples of deaerated and aerated perfuluorotributylamine (FC-43) were also irradiated with {sup 60}Co gamma rays (96 Gy/min) to various doses. The samples were extracted with NaOH and analyzed by IC and showed the presence of F and Cl{sup -}. The G-values were established. In surface study experiments Pu coupons were exposed to deaerated and aerated solutions of FC-43 and analyzed by X-ray photoelectron spectroscopy (XPS). The XPS data indicate that there is no detectable surface effect caused by the new fluid. In conclusion the FC-43 was determined to be a very effective and practical fluid for Pu density measurements.

  17. Ultra-trace determination of plutonium in marine samples using multi-collector inductively coupled plasma mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Lindahl, Patric, E-mail: patriclindahl@yahoo.com [Marine Environment Research Department, Korea Ocean Research and Development Institute, 1270 Sadong, Ansan 426-744 (Korea, Republic of); School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL48AA (United Kingdom); Keith-Roach, Miranda; Worsfold, Paul [School of Geography, Earth and Environmental Sciences, University of Plymouth, Drake Circus, Plymouth PL48AA (United Kingdom); Choi, Min-Seok; Shin, Hyung-Seon [Division of Earth and Environmental Science, Korea Basic Science Institute, 113 Gwahangno, Yusung-gu, Daejon 305-333 (Korea, Republic of); Lee, Sang-Hoon [Marine Geology and Geophysics Laboratory, Korea Ocean Research and Development Institute, 1270 Sadong, Ansan 426-744 (Korea, Republic of)

    2010-06-25

    Sources of plutonium isotopes to the marine environment are well defined, both spatially and temporally, which makes Pu a potential tracer for oceanic processes. This paper presents the selection, optimisation and validation of a sample preparation method for the ultra-trace determination of Pu isotopes ({sup 240}Pu and {sup 239}Pu) in marine samples by multi-collector (MC) ICP-MS. The method was optimised for the removal of the interference from {sup 238}U and the chemical recovery of Pu. Comparison of various separation strategies using AG1-X8, TEVA, TRU, and UTEVA resins to determine Pu in marine calcium carbonate samples is reported. A combination of anion-exchange (AG1-X8) and extraction chromatography (UTEVA/TRU) was the most suitable, with a radiochemical Pu yield of 87 {+-} 5% and a U decontamination factor of 1.2 x 10{sup 4}. Validation of the method was accomplished by determining Pu in various IAEA certified marine reference materials. The estimated MC-ICP-MS instrumental limit of detection for {sup 239}Pu and {sup 240}Pu was 0.02 fg mL{sup -1}, with an absolute limit of quantification of 0.11 fg. The proposed method allows the determination of ultra-trace Pu, at femtogram levels, in small size marine samples (e.g., 0.6-2.0 g coral or 15-20 L seawater). Finally, the analytical method was applied to determining historical records of the Pu signature in coral samples from the tropical Northwest Pacific and {sup 239+240}Pu concentrations and {sup 240}Pu/{sup 239}Pu atom ratios in seawater samples as part of the 2008 GEOTRACES intercalibration exercise.

  18. Habit formation, surplus consumption and return predictability

    DEFF Research Database (Denmark)

    Engsted, Tom; Hyde, Stuart; Vinther Møller, Stig

    2010-01-01

    -varying risk-free rate. In addition, we analyze the predictive power of the surplus consumption ratio for future stock and bond returns. We find that, although there are important cross-country differences and economically significant pricing errors, for the majority of countries in our sample the model gets...... empirical support in a variety of different dimensions, including reasonable estimates of risk-free rates. Further, for the majority of countries the surplus consumption ratio captures time-variation in expected returns. Together with the price-dividend ratio, the surplus consumption ratio contains...... significant information about future stock returns, also during the 1990s. In addition, in most countries the surplus consumption ratio is also a powerful predictor of future bond returns. Thus, the surplus consumption ratio captures time-varying expected returns in both stock and bond markets....

  19. Plutonium as a tracer for soil erosion assessment in northeast China.

    Science.gov (United States)

    Xu, Yihong; Qiao, Jixin; Pan, Shaoming; Hou, Xiaolin; Roos, Per; Cao, Liguo

    2015-04-01

    Soil erosion is one of the most serious environmental and agricultural problems faced by human society. Assessing intensity is an important issue for controlling soil erosion and improving eco-environmental quality. The suitability of the application of plutonium (Pu) as a tracer for soil erosion assessment in northeast China was investigated by comparing with that of 137Cs. Here we build on preliminary work, in which we investigated the potential of Pu as a soil erosion tracer by sampling additional reference sites and potential erosive sites, along the Liaodong Bay region in northeast China, for Pu isotopes and 137Cs. 240Pu/239Pu atomic ratios in all samples were approximately 0.18, which indicated that the dominant source of Pu was the global fallout. Pu showed very similar distribution patterns to those of 137Cs at both uncultivated and cultivated sites. 239+240Pu concentrations in all uncultivated soil cores followed an exponential decline with soil depth, whereas at cultivated sites, Pu was homogenously distributed in plow horizons. Factors such as planted crop types, as well as methods and frequencies of irrigation and tillage were suggested to influence the distribution of radionuclides in cultivated land. The baseline inventories of 239+240Pu and 137Cs were 88.4 and 1688 Bq m(-2) respectively. Soil erosion rates estimated by 239+240Pu tracing method were consistent with those obtained by the 137Cs method, confirming that Pu is an effective tracer with a similar tracing behavior to that of 137Cs for soil erosion assessment.

  20. Integrated development and testing plan for the plutonium immobilization project

    Energy Technology Data Exchange (ETDEWEB)

    Kan, T.

    1998-07-01

    This integrated plan for the DOE Office of Fissile Materials Disposition (MD) describes the technology development and major project activities necessary to support the deployment of the immobilization approach for disposition of surplus weapons-usable plutonium. The plan describes details of the development and testing (D&T) tasks needed to provide technical data for design and operation of a plutonium immobilization plant based on the ceramic can-in-canister technology (''Immobilization Fissile Material Disposition Program Final Immobilization Form Assessment and Recommendation'', UCRL-ID-128705, October 3, 1997). The plan also presents tasks for characterization and performance testing of the immobilization form to support a repository licensing application and to develop the basis for repository acceptance of the plutonium form. Essential elements of the plant project (design, construction, facility activation, etc.) are described, but not developed in detail, to indicate how the D&T results tie into the overall plant project. Given the importance of repository acceptance, specific activities to be conducted by the Office of Civilian Radioactive Waste Management (RW) to incorporate the plutonium form in the repository licensing application are provided in this document, together with a summary of how immobilization D&T activities provide input to the license activity. The ultimate goal of the Immobilization Project is to develop, construct, and operate facilities that will immobilize from about 18 to 50 tonnes (MT) of U.S. surplus weapons usable plutonium materials in a manner that meets the ''spent fuel'' standard (Fissile Materials Storage and Disposition Programmatic Environmental Impact Statement Record of Decision, ''Storage and Disposition Final PEIS'', issued January 14, 1997, 62 Federal Register 3014) and is acceptable for disposal in a geologic repository. In the can-in-canister technology

  1. The Association of Inbreeding With Lung Fibrosis Incidence in Beagle Dogs That Inhaled 238PuO2 or 239PuO2.

    Energy Technology Data Exchange (ETDEWEB)

    Wilson, Dulaney A.; Brigantic, Andrea M.; Morgan, William F.

    2011-09-12

    Studies of health effects in animals after exposure to internally deposited radionuclides were intended to supplement observational studies in humans. Both nuclear workers and Beagle dogs have exhibited plutonium associated lung fibrosis; however, the dogs smaller gene pool may limit the applicability of findings to humans. Data on Beagles that inhaled either plutonium-238 dioxide (238PuO2) or plutonium-239 dioxide (239PuO2) were analyzed. Wright's Coefficient of Inbreeding was used to measure genetic or familial susceptibility and was assessed as an explanatory variable when modeling the association between lung fibrosis incidence and plutonium exposure. Lung fibrosis was diagnosed in approximately 80% of the exposed dogs compared with 23.7% of the control dogs. The maximum degree of inbreeding was 9.4%. Regardless of isotope, the addition of inbreeding significantly improved the model in female dogs but not in males. In female dogs an increased inbreeding coefficient predicted decreased hazard of a lung fibrosis diagnosis. Lung fibrosis was common in these dogs with inbreeding affecting models of lung fibrosis incidence in females but not in males. The apparent protective effect in females predicted by these models of lung fibrosis incidence is likely to be minimal given the small degree of inbreeding in these groups.

  2. Isotopic and elemental composition of plutonium/americium oxides influence pulmonary and extra-pulmonary distribution after inhalation in rats.

    Science.gov (United States)

    Van der Meeren, A; Grémy, O

    2010-09-01

    The biodistribution of plutonium and americium has been studied in a rat model after inhalation of two PuO(2) powders in lungs and extra-pulmonary organs from 3 d to 3 mo. The main difference between the two powders was the content of americium (approximately 46% and 4.5% of total alpha activity). The PuO(2) with a higher proportion of americium shows an accelerated transfer of activity from lungs to blood as compared to PuO(2) with the lower americium content, illustrated by increased urinary excretion and higher bone and liver actinide retention. The total alpha activity measured reflects mostly the americium biological behavior. The activity contained in epithelial lining fluid, recovered in the acellular phase of broncho-alveolar lavages, mainly contains americium, whereas plutonium remains trapped in macrophages. Epithelial lining fluid could represent a transitional pulmonary compartment prior to translocation of actinides to the blood and subsequent deposition in extra-pulmonary retention organs. In addition, differential behaviors of plutonium and americium are also observed between the PuO(2) powders with a higher dissolution rate for both plutonium and americium being obtained for the PuO(2) with the highest americium content. Our results indicate that the biological behavior of plutonium and americium after translocation into blood differ two-fold: (1) for the two actinides for the same PuO(2) aerosol, and (2) for the same actinide from the two different aerosols. These results highlight the importance of considering the specific behavior of each contaminant after accidental pulmonary intake when assessing extra-pulmonary deposits from the level of activity excreted in urine or for therapeutic strategy decisions.

  3. Trench 'bathtubbing' and surface plutonium contamination at a legacy radioactive waste site.

    Science.gov (United States)

    Payne, Timothy E; Harrison, Jennifer J; Hughes, Catherine E; Johansen, Mathew P; Thiruvoth, Sangeeth; Wilsher, Kerry L; Cendón, Dioni I; Hankin, Stuart I; Rowling, Brett; Zawadzki, Atun

    2013-01-01

    Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (~12 Bq/L of (239+240)Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest (239+240)Pu soil activity was 829 Bq/kg in a shallow sample (0-1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the 'bathtub' effect.

  4. Trench ‘Bathtubbing’ and Surface Plutonium Contamination at a Legacy Radioactive Waste Site

    Science.gov (United States)

    2013-01-01

    Radioactive waste containing a few grams of plutonium (Pu) was disposed between 1960 and 1968 in trenches at the Little Forest Burial Ground (LFBG), near Sydney, Australia. A water sampling point installed in a former trench has enabled the radionuclide content of trench water and the response of the water level to rainfall to be studied. The trench water contains readily measurable Pu activity (∼12 Bq/L of 239+240Pu in 0.45 μm-filtered water), and there is an associated contamination of Pu in surface soils. The highest 239+240Pu soil activity was 829 Bq/kg in a shallow sample (0–1 cm depth) near the trench sampling point. Away from the trenches, the elevated concentrations of Pu in surface soils extend for tens of meters down-slope. The broader contamination may be partly attributable to dispersion events in the first decade after disposal, after which a layer of soil was added above the trenched area. Since this time, further Pu contamination has occurred near the trench-sampler within this added layer. The water level in the trench-sampler responds quickly to rainfall and intermittently reaches the surface, hence the Pu dispersion is attributed to saturation and overflow of the trenches during extreme rainfall events, referred to as the ‘bathtub’ effect. PMID:24256473

  5. Dispersion stability and electrokinetic properties of intrinsic plutonium colloids: implications for subsurface transport.

    Science.gov (United States)

    Abdel-Fattah, Amr I; Zhou, Dongxu; Boukhalfa, Hakim; Tarimala, Sowmitri; Ware, S Doug; Keller, Arturo A

    2013-06-04

    Subsurface transport of plutonium (Pu) may be facilitated by the formation of intrinsic Pu colloids. While this colloid-facilitated transport is largely governed by the electrokinetic properties and dispersion stability (resistance to aggregation) of the colloids, reported experimental data is scarce. Here, we quantify the dependence of ζ-potential of intrinsic Pu(IV) colloids on pH and their aggregation rate on ionic strength. Results indicate an isoelectric point of pH 8.6 and a critical coagulation concentration of 0.1 M of 1:1 electrolyte at pH 11.4. The ζ-potential/pH dependence of the Pu(IV) colloids is similar to that of goethite and hematite colloids. Colloid interaction energy calculations using these values reveal an effective Hamaker constant of the intrinsic Pu(IV) colloids in water of 1.85 × 10(-19) J, corresponding to a relative permittivity of 6.21 and refractive index of 2.33, in agreement with first principles calculations. This relatively high Hamaker constant combined with the positive charge of Pu(IV) colloids under typical groundwater aquifer conditions led to two contradicting hypotheses: (a) the Pu(IV) colloids will exhibit significant aggregation and deposition, leading to a negligible subsurface transport or (b) the Pu(IV) colloids will associate with the relatively stable native groundwater colloids, leading to a considerable subsurface transport. Packed column transport experiments supported the second hypothesis.

  6. Performance characteristics of a Bioassay method for plutonium using thermal ionisation mass spectrometry (TIMS)

    Energy Technology Data Exchange (ETDEWEB)

    Linauskas, S.H.; Elliot, N.L.; Paterson, L.M.; Totland, M.M

    2003-01-01

    Plutonium-in-urine analysis by radiochemical isolation of Pu followed by thermal ionisation mass spectrometry (TIMS) is capable of high sensitivity and precision measurements {sup 239}Pu and {sup 240}Pu. Bias and precision estimates for the TIMS bioassay program at Chalk River Laboratories easily met the ANSI N13.30 performance criteria standards with {sup 239}Pu results of 1.5% and 3.0%, respectively. Analytical blanks derived from water, artificial urine and true urine samples did not produce any statistically different results. During a four-year period of development and implementation of {sup 239}Pu measurements by TIMS, average sample blank values were reduced from 3.9 fg (9.0 {mu}Bq) to 0.57 fg (1.3 {mu}Bq). This reduction was achieved through rigorous application of clean-room handling techniques throughout sample processing. Blank data were found to follow a Iognormal distribution, and current detection limit parameters for L{sub c} and L{sub d} at the 95% significance levels are 0.85 fg {sup 239}Pu (2.0 {mu}Bq) and 1.3 fg {sup 239}Pu (3.0 {mu}Bq), respectively. Detection limits in this range are expected to be sufficient to identify intakes of Pu/Am mixtures at levels that are around one-twentieth of an ALl or better under routine monitoring situations for ICRP Type S and Type M inhalation solubility classes. (author)

  7. ZPR-6 assembly 7 high {sup 240}Pu core experiments : a fast reactor core with mixed (Pu,U)-oxide fuel and a centeral high{sup 240}Pu zone.

    Energy Technology Data Exchange (ETDEWEB)

    Lell, R. M.; Morman, J. A.; Schaefer, R.W.; McKnight, R.D.; Nuclear Engineering Division

    2009-02-23

    ZPR-6 Assembly 7 (ZPR-6/7) encompasses a series of experiments performed at the ZPR-6 facility at Argonne National Laboratory in 1970 and 1971 as part of the Demonstration Reactor Benchmark Program (Reference 1). Assembly 7 simulated a large sodium-cooled LMFBR with mixed oxide fuel, depleted uranium radial and axial blankets, and a core H/D near unity. ZPR-6/7 was designed to test fast reactor physics data and methods, so configurations in the Assembly 7 program were as simple as possible in terms of geometry and composition. ZPR-6/7 had a very uniform core assembled from small plates of depleted uranium, sodium, iron oxide, U{sub 3}O{sub 8} and Pu-U-Mo alloy loaded into stainless steel drawers. The steel drawers were placed in square stainless steel tubes in the two halves of a split table machine. ZPR-6/7 had a simple, symmetric core unit cell whose neutronic characteristics were dominated by plutonium and {sup 238}U. The core was surrounded by thick radial and axial regions of depleted uranium to simulate radial and axial blankets and to isolate the core from the surrounding room. The ZPR-6/7 program encompassed 139 separate core loadings which include the initial approach to critical and all subsequent core loading changes required to perform specific experiments and measurements. In this context a loading refers to a particular configuration of fueled drawers, radial blanket drawers and experimental equipment (if present) in the matrix of steel tubes. Two principal core configurations were established. The uniform core (Loadings 1-84) had a relatively uniform core composition. The high {sup 240}Pu core (Loadings 85-139) was a variant on the uniform core. The plutonium in the Pu-U-Mo fuel plates in the uniform core contains 11% {sup 240}Pu. In the high {sup 240}Pu core, all Pu-U-Mo plates in the inner core region (central 61 matrix locations per half of the split table machine) were replaced by Pu-U-Mo plates containing 27% {sup 240}Pu in the plutonium

  8. Nonreversible immobilization of water-borne plutonium onto self-assembled adlayers of silanized humic materials.

    Science.gov (United States)

    Shcherbina, Natalia S; Kalmykov, Stepan S; Karpiouk, Leonid A; Ponomarenko, Sergey A; Hatfield, Kirk; Haire, Richard; Perminova, Irina V

    2014-02-18

    The objective was to study plutonium partitioning between immobile and mobile humic materials at the water-solid interfaces. Immobilization of the humic materials on solid supports was performed in situ using self-adhesive silanized humic derivatives. The presence of the humic adlayers on solid supports was shown to significantly enhance Pu sorption and its retention under both steady state and dynamic conditions. While plutonium may exist in multiple oxidations states plus colloidal forms, the major thrust in this work was to study the behavior of most mobile--the PuO2(+) form in dilute solutions. The values of the plutonium partition coefficients (Kd) between water and humics-coated silica gels after 10 days exposure reached 1.6 × 10(4) L · kg(-1) at pH 7.5 under anaerobic conditions with a total plutonium concentration of 1.2 × 10(-8) M exceeding those for the uncoated SiO2 (6.3 × 10(2) L · kg(-1)). Column tests showed substantial sequestration of water-borne plutonium (up to 73%) on the humics-coated silica gels. Remobilization experiments conducted under batch conditions at different pH values (3.5, 4.5, 7.5) showed that no more than 3% of the sequestered Pu was remobilized from the humics-coated silica gels by treatment with dissolved humic materials at environmentally relevant pH of 7.5. Consequently, silanized humic materialas can be seen as both molecular probes and as potent candidate materials for scavenging mobile Pu from an aqueous phase.

  9. Plutonium and Minor Actinides Recycling in Standard BWR using Equilibrium Burnup Model

    Directory of Open Access Journals (Sweden)

    Abdul Waris

    2008-03-01

    Full Text Available Plutonium (Pu and minor actinides (MA recycling in standard BWR with equilibrium burnup model has been studied. We considered the equilibrium burnup model as a simple time independent burnup method, which can manage all possible produced nuclides in any nuclear system. The equilibrium burnup code was bundled with a SRAC cell-calculation code to become a coupled cell-burnup calculation code system. The results show that the uranium enrichment for the criticality of the reactor, the amount of loaded fuel and the required natural uranium supply per year decrease for the Pu recycling and even much lower for the Pu & MA recycling case compared to those of the standard once-through BWR case. The neutron spectra become harder with the increasing number of recycled heavy nuclides in the reactor core. The total fissile rises from 4.77% of the total nuclides number density in the reactor core for the standard once-through BWR case to 6.64% and 6.72% for the Plutonium recycling case and the Pu & MA recycling case, respectively. The two later data may become the main basis why the required uranium enrichment declines and consequently diminishes the annual loaded fuel and the required natural uranium supply. All these facts demonstrate the advantage of plutonium and minor actinides recycling in BWR.

  10. Interaction of Plutonium with Bacteria in the Repository Environment

    Energy Technology Data Exchange (ETDEWEB)

    Gillow, J. B.; Francis, A. J.; Lucero, D. A.; Papenguth, H. W.

    2000-07-01

    Microorganisms in the nuclear waste repository environment may interact with plutonium through (1) sorption, (2) intracellular accumulation, and (3) transformation speciation. These interactions may retard or enhance the mobility of Pu by precipitation reactions, biocolloid formation, or production of more soluble species. Current and planned radioactive waste repository environments, such as deep subsurface halite and granite formations, are considered extreme relative to life processes in the near-surface terrestrial environment. There is a paucity of information on the biotransformation of radionuclides by microorganisms present in such extreme environments. In order to gain a better understanding of the interaction of plutonium with microorganisms present in the waste repository sites we investigated a pure culture (Halomonas sp.) and a mixed culture of bacteria (Haloarcula sinaiiensis, Marinobacter hydrocarbonoclasticus, Altermonas sp., and a {gamma}-proteobacterium) isolated from the Waste Isolation Pilot Plant (WIPP) site and an Acetobacterium sp. from alkaline groundwater at the Grimsel Test Site in Switzerland.

  11. Plutonium as a tracer for soil erosion assessment in northeast China

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Yihong [School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023 (China); Qiao, Jixin [Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, DK-4000 Roskilde (Denmark); Pan, Shaoming, E-mail: span@nju.edu.cn [School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023 (China); Hou, Xiaolin, E-mail: xiho@dtu.dk [Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, DK-4000 Roskilde (Denmark); Xi' an AMS Center, SKLLQG, Institute of Earth Environment, CAS, Xi' an 710075 (China); Roos, Per [Center for Nuclear Technologies, Technical University of Denmark, Risø Campus, DK-4000 Roskilde (Denmark); Cao, Liguo [School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023 (China)

    2015-04-01

    Soil erosion is one of the most serious environmental and agricultural problems faced by human society. Assessing intensity is an important issue for controlling soil erosion and improving eco-environmental quality. The suitability of the application of plutonium (Pu) as a tracer for soil erosion assessment in northeast China was investigated by comparing with that of {sup 137}Cs. Here we build on preliminary work, in which we investigated the potential of Pu as a soil erosion tracer by sampling additional reference sites and potential erosive sites, along the Liaodong Bay region in northeast China, for Pu isotopes and {sup 137}Cs. {sup 240}Pu/{sup 239}Pu atomic ratios in all samples were approximately 0.18, which indicated that the dominant source of Pu was the global fallout. Pu showed very similar distribution patterns to those of {sup 137}Cs at both uncultivated and cultivated sites. {sup 239+240}Pu concentrations in all uncultivated soil cores followed an exponential decline with soil depth, whereas at cultivated sites, Pu was homogenously distributed in plow horizons. Factors such as planted crop types, as well as methods and frequencies of irrigation and tillage were suggested to influence the distribution of radionuclides in cultivated land. The baseline inventories of {sup 239+240}Pu and {sup 137}Cs were 88.4 and 1688 Bq m{sup −2} respectively. Soil erosion rates estimated by {sup 239+240}Pu tracing method were consistent with those obtained by the {sup 137}Cs method, confirming that Pu is an effective tracer with a similar tracing behavior to that of {sup 137}Cs for soil erosion assessment. - Highlights: • The potential for the use of Pu as a soil erosion tracer was investigated. • Pu would be a good tracer given its long half-life. • Depth profiles of Pu in soils were systematically studied and compared to {sup 137}Cs. • Pu is an effective soil erosion tracer with behavior similar to that of {sup 137}Cs. • Thus, Pu provides a means of

  12. An iron-dependent and transferrin-mediated cellular uptake pathway for plutonium.

    Energy Technology Data Exchange (ETDEWEB)

    Jensen, M. P.; Gorman-Lewis, D.; Aryal, B. P.; Paunesku, T.; Vogt, S.; Rickert, P. G.; Seifert, S.; Lai, B.; Woloschak, G. E.; Soderholm, L. (Chemical Sciences and Engineering Division); ( XSD); (Univ. of Chicago); (Northwestern Univ.)

    2011-08-01

    Plutonium is a toxic synthetic element with no natural biological function, but it is strongly retained by humans when ingested. Using small-angle X-ray scattering, receptor binding assays and synchrotron X-ray fluorescence microscopy, we find that rat adrenal gland (PC12) cells can acquire plutonium in vitro through the major iron acquisition pathway -- receptor-mediated endocytosis of the iron transport protein serum transferrin; however, only one form of the plutonium-transferrin complex is active. Low-resolution solution models of plutonium-loaded transferrins derived from small-angle scattering show that only transferrin with plutonium bound in the protein's C-terminal lobe (C-lobe) and iron bound in the N-terminal lobe (N-lobe) (Pu{sub c}Fe{sub N}Tf) adopts the proper conformation for recognition by the transferrin receptor protein. Although the metal-binding site in each lobe contains the same donors in the same configuration and both lobes are similar, the differences between transferrin's two lobes act to restrict, but not eliminate, cellular Pu uptake.

  13. An iron-dependent and transferrin-mediated cellular uptake pathway for plutonium.

    Science.gov (United States)

    Jensen, Mark P; Gorman-Lewis, Drew; Aryal, Baikuntha; Paunesku, Tatjana; Vogt, Stefan; Rickert, Paul G; Seifert, Soenke; Lai, Barry; Woloschak, Gayle E; Soderholm, L

    2011-06-26

    Plutonium is a toxic synthetic element with no natural biological function, but it is strongly retained by humans when ingested. Using small-angle X-ray scattering, receptor binding assays and synchrotron X-ray fluorescence microscopy, we find that rat adrenal gland (PC12) cells can acquire plutonium in vitro through the major iron acquisition pathway--receptor-mediated endocytosis of the iron transport protein serum transferrin; however, only one form of the plutonium-transferrin complex is active. Low-resolution solution models of plutonium-loaded transferrins derived from small-angle scattering show that only transferrin with plutonium bound in the protein's C-terminal lobe (C-lobe) and iron bound in the N-terminal lobe (N-lobe) (Pu(C)Fe(N)Tf) adopts the proper conformation for recognition by the transferrin receptor protein. Although the metal-binding site in each lobe contains the same donors in the same configuration and both lobes are similar, the differences between transferrin's two lobes act to restrict, but not eliminate, cellular Pu uptake.

  14. Pu在地质介质中的分配系数及影响因素分析%Distribution Coefficient of Plutonium on Geological Medium and Factor Effect

    Institute of Scientific and Technical Information of China (English)

    于静; 司高华; 黄云贵; 刘勇; 贾海红; 郑军芳; 王旭辉

    2011-01-01

    The distribution coefficients of Pu(Ⅳ ) and Pu( Ⅴ ) between aeolian sand, sandy soil, or gravel soil and water, and of Pu(Ⅴ ) between iron or iron oxides and water were determined with batch experiments. Various factors that affect the plutonium sorption were examined, including the soil composition, the oxidation state of Pu, and the method for preparation of Pu spike solutions. The sorption of Pu(Ⅳ) in soil is found more stronger than that of Pu( Ⅴ ). Their distribution coefficients in clayey silt are in the range of 103-104 mL/g, while those of Pu( Ⅴ ) in iron oxides reach as high as 105-106 mL/g. A higher clay content in clayey silt favarites the sorption of plutonium. The method for preparation of Pu spike solutions also influences the distribution coefficient of plutonium even all other experimental conditions are kept unchanged.%用静态法实验测定了Pu(Ⅳ)和Pu(Ⅴ)在风积沙、沙黄土、沙砾石、铁及其氧化物中的分配系数,比较了Pu(Ⅳ)和Pu(Ⅴ)在几种介质上的吸附性能,并采用两种不同的Pu(Ⅳ)示踪液制备方法测定Pu(Ⅳ)在风积沙、沙黄土、沙砾石上的分配系数.结果表明,Pu(Ⅳ)和Pu(Ⅴ)在砂土中的分配系数为103~104 mL/g量级,Pu(Ⅴ)在铁及其氧化物中的分配系数为105~106mL/g量级,铁氧化物介质对Pu的吸附性最强,其次为粘土矿物含量大的介质;Pu(Ⅳ)比Pu(Ⅴ)更强的吸附在砂土上;Pu(Ⅳ)示踪液的制备采用两种不同方法时,在制备过程中Pu(Ⅳ)形成的化合物不同,其在砂土上的分配系数会随之不同.

  15. PLUTONIUM SOLUBILITY IN SIMULATED SAVANNAH RIVER SITE WASTE SOLUTIONS

    Energy Technology Data Exchange (ETDEWEB)

    Rudisill, T.; Hobbs, D.; Edwards, T.

    2010-09-27

    To address the accelerated disposition of the supernate and salt portions of Savannah River Site (SRS) high level waste (HLW), solubility experiments were performed to develop a predictive capability for plutonium (Pu) solubility. A statistically designed experiment was used to measure the solubility of Pu in simulated solutions with salt concentrations and temperatures which bounded those observed in SRS HLW solutions. Constituents of the simulated waste solutions included: hydroxide (OH{sup -}), aluminate (Al(OH){sub 4}{sup -}), sulfate (SO{sub 4}{sup 2-}), carbonate (CO{sub 3}{sup 2-}), nitrate (NO{sub 3}{sup -}), and nitrite (NO{sub 2}{sup -}) anions. Each anion was added to the waste solution in the sodium form. The solubilities were measured at 25 and 80 C. Five sets of samples were analyzed over a six month period and a partial sample set was analyzed after nominally fifteen months of equilibration. No discernable time dependence of the measured Pu concentrations was observed except for two salt solutions equilibrated at 80 C which contained OH{sup -} concentrations >5 mol/L. In these solutions, the Pu solubility increased with time. This observation was attributed to the air oxidation of a portion of the Pu from Pu(IV) to the more soluble Pu(V) or Pu(VI) valence states. A data driven approach was subsequently used to develop a modified response surface model for Pu solubility. Solubility data from this study and historical data from the literature were used to fit the model. The model predicted the Pu solubility of the solutions from this study within the 95% confidence interval for individual predictions and the analysis of variance indicated no statistically significant lack of fit. The Savannah River National Laboratory (SRNL) model was compared with predicted values from the Aqueous Electrolyte (AQ) model developed by OLI Systems, Inc. and a solubility prediction equation developed by Delegard and Gallagher for Hanford tank waste. The agreement between

  16. The Role of Colloids in the Transport of Plutonium and Americium: Implications for

    Energy Technology Data Exchange (ETDEWEB)

    Kersting, A B

    2003-09-17

    Colloids are small particulates (ranging in size from 1 to 0.001 micron) composed of inorganic and organic material and found in all natural water. Due to their small size, they have the ability to remain suspended in water and transported. Small amounts of plutonium (Pu) and americium (Am) can adsorb (attach) to colloids, and/or form colloidal-sized polymers and migrate in water. At Rocky Flats Environmental Technology Site (RFETS) sedimentation and resuspension of particulates and colloids in surface waters represent the dominant process for Pu and Am migration. The amount of Pu and Am that can be transported at RFETS has been quantified in the Pathway Analysis Report. The Pathway Analysis Report shows that the two dominant pathways for Pu and Am transport at RFETS are air and surface water. Shallow groundwater and biological pathways are minor.

  17. Combined exposure of F344 rats to beryllium metal and plutonium-239 dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Finch, G.L.; Carlton, W.W.; Rebar, A.H. [Purdue Univ., Lafayette, IN (United States)] [and others

    1995-12-01

    Nuclear weapons industry workers have the potential for inhalation exposures to plutonium (Pu) and other agents, such as beryllium (Be) metal. The purpose of this ongoing study is to investigate potential interactions between Pu and Be in the production of lung tumors in rats exposed by inhalation to particles of {sup 239}PuO{sub 2}, Be metal, or these agents in combination. Inhaled Pu deposited in the lung delivers high-linear-energy transfer, alpha-particle radiation and is known to induce pulmonary cancer in laboratory animals. Although the epidemiological evidence implicating Be in the induction of human lung cancer is weak and controversial, various studies in laboratory animals have demonstrated the pulmonary carcinogenicity of Be. As a result, Be is classified as a suspect human carcinogen in the United STates and as a demonstrated human carcinogen by the International Agency for Research on Cancer. This study is in progress.

  18. The Distribution of Plutonium(Ⅲ,Ⅳ) Nitrate Between Dilute TBP/OK and Aqueous Phase

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    The distribution of plutonium (Ⅲ, Ⅳ) nitrate between dilute TBP/OK and aqueous phase is systematically investigated. On the basis of the preparation and stabilization of Pu(Ⅲ, Ⅳ), the influences of the concentration of HNO3, Al(NO3)3, TBP and UO2(NO3)2 on the distribution ratio of them are studied at 25℃. The results indicate that the distribution ratio of Pu(Ⅳ) has a maximum while that of Pu(Ⅲ) increases with the concentration of HNO3. The distribution ratio of Pu(Ⅲ, Ⅳ) increases along with the concentration of Al(NO3)3 and TBP. The extraction reaction

  19. The production of {sup 238-242}Pu(n,γ){sup 239-243}Pu fissionable fluids in a fusion-fission hybrid reactor

    Energy Technology Data Exchange (ETDEWEB)

    Guenay, Mehtap [Inoenue Univ., Malatya (Turkey). Physics Dept.

    2014-03-15

    In this study, the effect of spent fuel grade plutonium content on {sup 239-243}Pu was investigated in a designed hybrid reactor system. In this system, the fluids were composed of a molten salt, heavy metal mixture with increased mole fractions 99-95 % Li{sub 20}Sn{sub 80}-1-5 % SFG-Pu, 99-95 % Li{sub 20}Sn{sub 80}-1-5 % SFG-PuF{sub 4}, 99-95 % Li{sub 20}Sn{sub 80}-1-5 % SFG-PuO{sub 2}. Beryllium (Be) is a neutron multiplier by (n,2n) reactions. Thence, a Be zone of 3 cm thickness was used in order to contribute to fissile fuel breeding between the liquid first wall and a 9Cr2WVTa ferritic steel blanket which is used as structural material. The production of {sup 238-242}Pu(n,γ){sup 239-243}Pu was calculated in liquid first wall, blanket and shielding zones. Three-dimensional nucleonic calculations were performed by using the most recent version MCNPX-2.7.0 Monte Carlo code and nuclear data library ENDF/B-VII.0. (orig.)

  20. Standard test method for 238Pu isotopic abundance by alpha spectrometry

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2001-01-01

    1.1 This test method covers the use of alpha spectrometry for determining the 238Pu isotopic abundance in plutonium samples. It is particularly useful for samples in which the 238Pu content is less than 1 % of the total plutonium content. For such samples, mass spectrometric results are less reliable than those from alpha spectrometry because of interference from any 238U isobar remaining after ion exchange. 1.2 This standard does not purport to address all of the safety concerns, if any, associated with its use. It is the responsibility of the user of this standard to establish appropriate safety and health practices and determine the applicability of regulatory limitations prior to use.

  1. Plutonium Finishing Plant. Interim plutonium stabilization engineering study

    Energy Technology Data Exchange (ETDEWEB)

    Sevigny, G.J.; Gallucci, R.H.; Garrett, S.M.K.; Geeting, J.G.H.; Goheen, R.S.; Molton, P.M.; Templeton, K.J.; Villegas, A.J. [Pacific Northwest Lab., Richland, WA (United States); Nass, R. [Nuclear Fuel Services, Inc. (United States)

    1995-08-01

    This report provides the results of an engineering study that evaluated the available technologies for stabilizing the plutonium stored at the Plutonium Finishing Plant located at the hanford Site in southeastern Washington. Further processing of the plutonium may be required to prepare the plutonium for interim (<50 years) storage. Specifically this document provides the current plutonium inventory and characterization, the initial screening process, and the process descriptions and flowsheets of the technologies that passed the initial screening. The conclusions and recommendations also are provided. The information contained in this report will be used to assist in the preparation of the environmental impact statement and to help decision makers determine which is the preferred technology to process the plutonium for interim storage.

  2. Sequential Injection Method for Rapid and Simultaneous Determination of 236U, 237Np, and Pu Isotopes in Seawater

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Steier, Peter;

    2013-01-01

    An automated analytical method implemented in a novel dual-column tandem sequential injection (SI) system was developed for simultaneous determination of 236U, 237Np, 239Pu, and 240Pu in seawater samples. A combination of TEVA and UTEVA extraction chromatography was exploited to separate and purify...... target analytes, whereupon plutonium and neptunium were simultaneously isolated and purified on TEVA, while uranium was collected on UTEVA. The separation behavior of U, Np, and Pu on TEVA–UTEVA columns was investigated in detail in order to achieve high chemical yields and complete purification...... for the radionuclides of interest. 242Pu was used as a chemical yield tracer for both plutonium and neptunium. 238U was quantified in the sample before the separation for deducing the 236U concentration from the measured 236U/238U atomic ratio in the separated uranium target using accelerator mass spectrometry...

  3. Disposition of PUREX facility tanks D5 and E6 uranium and plutonium solutions. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Harty, D.P.

    1993-12-01

    Approximately 9 kilograms of plutonium and 5 metric tons of uranium in a 1 molar nitric acid solution are being stored in two PUREX facility vessels, tanks D5 and E6. The plutonium was accumulated during cleanup activities of the plutonium product area of the PUREX facility. Personnel at PUREX recently completed a formal presentation to the Surplus Materials Peer Panel (SMPP) regarding disposition of the material currently in these tanks. The peer panel is a group of complex-wide experts who have been chartered by EM-64 (Office of Site and Facility Transfer) to provide a third party independent review of disposition decisions. The information presented to the peer panel is provided in the first section of this report. The panel was generally receptive to the information provided at that time and the recommendations which were identified.

  4. U.S. weapons-usable plutonium disposition policy: Implementation of the MOX fuel option

    Energy Technology Data Exchange (ETDEWEB)

    Woods, A.L. [ed.] [Amarillo National Resource Center for Plutonium, TX (United States); Gonzalez, V.L. [Texas A and M Univ., College Station, TX (United States). Dept. of Political Science

    1998-10-01

    A comprehensive case study was conducted on the policy problem of disposing of US weapons-grade plutonium, which has been declared surplus to strategic defense needs. Specifically, implementation of the mixed-oxide fuel disposition option was examined in the context of national and international nonproliferation policy, and in contrast to US plutonium policy. The study reveals numerous difficulties in achieving effective implementation of the mixed-oxide fuel option including unresolved licensing and regulatory issues, technological uncertainties, public opposition, potentially conflicting federal policies, and the need for international assurances of reciprocal plutonium disposition activities. It is believed that these difficulties can be resolved in time so that the implementation of the mixed-oxide fuel option can eventually be effective in accomplishing its policy objective.

  5. Neptunium and plutonium complexes with a sterically encumbered triamidoamine (TREN) scaffold.

    Science.gov (United States)

    Brown, Jessie L; Gaunt, Andrew J; King, David M; Liddle, Stephen T; Reilly, Sean D; Scott, Brian L; Wooles, Ashley J

    2016-04-07

    The syntheses and characterisation of isostructural neptunium(iv) and plutonium(iv) complexes [An(IV)(TREN(TIPS))(Cl)] [An = Np, Pu; TREN(TIPS) = {N(CH2CH2NSiPr(i)3)3}(3-)] are reported, along with the demonstration that they are likely reduced to the corresponding neptunium(iii) and plutonium(iii) products [An(III)(TREN(TIPS))]; this chemistry provides new platforms from which to target a plethora of unprecedented molecular functionalities in transuranic chemistry and the neptunium(iv) molecule is the first structurally characterised neptunium(iv)-amide complex.

  6. Determination of thorium in plutonium-thorium oxides and carbides

    Energy Technology Data Exchange (ETDEWEB)

    Walker, L.F.; Temer, D.J.

    1979-10-01

    Thorium is determined in (PuTh)C and (PuTh)O/sub 2/ by complexometric titration with ethylenediaminetetraacetic acid (EDTA) following separation on anion-exchange resin. Carbides are first oxidized by ignition in air at about 800/sup 0/C. Oxide or oxidized carbide samples are dissolved in acids by the sealed-reflux technique or by heating in beakers. The plutonium is selectively sorbed from the 12M hydrochloric acid solution of the fuel on a Bio-Rad AG1-X2 anion-exchange resin column, and the eluted thorium is titrated with EDTA using xylenol orange as the indicator. The average recovery of thorium in 20 samples is 99.98% with a relative standard deviation of 0.07%.

  7. Plutonium-244 fission xenon in the most primitive meteorites

    Energy Technology Data Exchange (ETDEWEB)

    Kuroda, P.K.; Myers, W.A. (Dept. of Chemical Engineering, Univ. Arkansas, Fayetteville, AR (United States))

    1994-01-01

    The plutonium-244/xenon-136 ages of the Murchison, Murray and Orgueil meteorites have been calculated from the existing xenon isotope data and the uranium contents. The CI carbonaceous chondrite Orgueil, which is considered to be among the most primitive - in the sense of the least altered - sample of the solar system known to man, appears to have started to retain its xenon more than 5,000 million years ago, when the ratio of [sup 244]Pu to [sup 238]U in the solar system was as high as (0.5 [+-] 0.1) (atom/atom) and the CM carbonaceous chondrites Murchison and Murray started to retain their xenon about 4,940 million years ago, when the [sup 244]Pu to [sup 238]U ratio was about 0.17 (atom/atom). (orig.)

  8. Biodegradation of PuEDTA and Impacts on Pu Mobility

    Energy Technology Data Exchange (ETDEWEB)

    Bolton, H., Jr.; Rai, D.; Xun, L.

    2004-03-17

    The contamination of many DOE sites by Pu presents a long-term problem because of its long half-life (240,000 yrs) and the low drinking water standard (<10{sup -12} M). EDTA was co-disposed with radionuclides (e.g., Pu, {sup 60}Co), formed strong complexes, and enhanced radionuclide transport at several DOE sites. Biodegradation of EDTA should decrease Pu mobility. One objective of this project was to determine the biodegradation of EDTA in the presence of PuEDTA complexes. The aqueous system investigated at pH 7 (10{sup -4} M EDTA and 10{sup -6} M Pu) contained predominantly Pu(OH){sub 2}EDTA{sup 2-}. The EDTA was degraded at a faster rate in the presence of Pu. As the total concentration of both EDTA and PuEDTA decreased (i.e., 10{sup -5} M EDTA and 10{sup -7} M PuEDTA), the presence of Pu decreased the biodegradation rate of the EDTA. It is currently unclear why the concentration of Pu directly affects the increase/decrease in rate of EDTA biodegradation. The soluble Pu concentration decreased, in agreement with thermodynamic predictions, as the EDTA was biodegraded, indicating that biodegradation of EDTA will decrease Pu mobility when the Pu is initially present as Pu(IV)EDTA. A second objective was to investigate how the presence of competing metals, commonly encountered in geologic media, will influence the speciation and biodegradation of Pu(IV)-EDTA. Studies on the solubilities of Fe(OH){sub 3}(s) and of Fe(OH){sub 3}(s) plus PuO{sub 2}(am) in the presence of EDTA and as a function of pH showed that Fe(III) out competes the Pu(IV) for the EDTA complex, thereby showing that Pu(IV) will not form stable complexes with EDTA for enhanced transport of Pu in Fe(III) dominated subsurface systems. A third objective is to investigate the genes and enzymes involved in EDTA biodegradation. BNC1 can use EDTA and another synthetic chelating agent nitrilotriacetate (NTA) as sole carbon and nitrogen sources. The same catabolic enzymes are responsible for both EDTA and NTA

  9. Hydrothermal Alteration of Glass from Underground Nuclear Tests: Formation and Transport of Pu-clay Colloids at the Nevada National Security Site

    Energy Technology Data Exchange (ETDEWEB)

    Zavarin, M. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Zhao, P. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Joseph, C. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Begg, J. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Boggs, M. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Dai, Z. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Kersting, A. B. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2015-05-27

    The testing of nuclear weapons at the Nevada National Security Site (NNSS), formerly the Nevada Test Site (NTS), has led to the deposition of substantial quantities of plutonium into the environment. Approximately 2.8 metric tons (3.1×104 TBq) of Pu were deposited in the NNSS subsurface as a result of underground nuclear testing. While 3H is the most abundant anthropogenic radionuclide deposited in the NNSS subsurface (4.7×106 TBq), plutonium is the most abundant from a molar standpoint. The only radioactive elements in greater molar abundance are the naturally occurring K, Th, and U isotopes. 239Pu and 240Pu represent the majority of alpha-emitting Pu isotopes. The extreme temperatures associated with underground nuclear tests and the refractory nature of Pu results in most of the Pu (98%) being sequestered in melted rock, referred to as nuclear melt glass (Iaea, 1998). As a result, Pu release to groundwater is controlled, in large part, by the leaching (or dissolution) of nuclear melt glass over time. The factors affecting glass dissolution rates have been studied extensively. The dissolution of Pu-containing borosilicate nuclear waste glasses at 90ºC has been shown to lead to the formation of dioctahedral smectite colloids. Colloid-facilitated transport of Pu at the NNSS has been observed. Recent groundwater samples collected from a number of contaminated wells have yielded a wide range of Pu concentrations from 0.00022 to 2.0 Bq/L. While Pu concentrations tend to fall below the Maximum Contaminant Level (MCL) established by the Environmental Protection Agency (EPA) for drinking water (0.56 Bq/L), we do not yet understand what factors limit the Pu concentration or its transport behavior. To quantify the upper limit of Pu concentrations produced as a result of melt glass dissolution and determine the nature of colloids and Pu associations, we performed a 3 year nuclear melt glass dissolution experiment

  10. Measurement of the 242Pu(n,f cross section at n_TOF

    Directory of Open Access Journals (Sweden)

    Tsinganis A.

    2014-03-01

    Full Text Available Knowledge of neutron cross sections of various plutonium isotopes and other minor actinides is crucial for the design of advanced nuclear systems. The 242Pu(n,f cross sections were measured at the CERN n_TOF facility, taking advantage of the wide energy range (from thermal to GeV and the high instantaneous flux of the neutron beam. In this work, preliminary results are presented along with a theoretical cross section calculation performed with the EMPIRE code.

  11. 45 CFR 12.7 - Applications for surplus real property.

    Science.gov (United States)

    2010-10-01

    ... 45 Public Welfare 1 2010-10-01 2010-10-01 false Applications for surplus real property. 12.7 Section 12.7 Public Welfare DEPARTMENT OF HEALTH AND HUMAN SERVICES GENERAL ADMINISTRATION DISPOSAL AND UTILIZATION OF SURPLUS REAL PROPERTY FOR PUBLIC HEALTH PURPOSES § 12.7 Applications for surplus real property. Applications for surplus real...

  12. EVALUATION OF IMPURITY EXTREMES IN A PLUTONIUM-LOADED BOROSILICATE GLASS

    Energy Technology Data Exchange (ETDEWEB)

    Marra, J; Kevin Fox, K; Charles Crawford, C; Ned Bibler, N; Elizabeth Hoffman, E; Tommy Edwards, T

    2007-11-12

    A vitrification technology utilizing a lanthanide borosilicate (LaBS) glass appears to be a viable option for the disposition of excess weapons-useable plutonium that is not suitable for processing into mixed oxide (MOX) fuel. A significant effort to develop a glass formulation and vitrification process to immobilize plutonium was completed in the mid-1990s. The LaBS glass formulation was found to be capable of immobilizing in excess of 10 wt % Pu and to be tolerant of a range of impurities. To confirm the results of previous testing with surrogate Pu feeds containing impurities, four glass compositions were selected for fabrication with actual plutonium oxide and impurities. The four compositions represented extremes in impurity type and concentration. The homogeneity and durability of these four compositions were measured. The homogeneity of the glasses was evaluated using x-ray diffraction (XRD) and scanning electron microscopy coupled with energy dispersive spectroscopy (SEM/EDS). The XRD results indicated that the glasses were amorphous with no evidence of crystalline species in the glass. The SEM/EDS analyses did show the presence of some undissolved PuO{sub 2} material. The EDS spectra indicated that some of the PuO{sub 2} crystals also contained hafnium oxide. The SEM/EDS analyses showed that there were no heterogeneities in the glass due to the feed impurities. The durability of the glasses was measured using the Product Consistency Test (PCT). The PCT results indicated that the durability of Pu impurity glasses was comparable with Pu glasses without impurities and significantly more durable than the Environmental Assessment (EA) glass used as the benchmark for repository disposition of high-level waste (HLW) glasses.

  13. Plutonium and americium in fish, shellfish and seaweed in the Irish environment and their contribution to dose

    Energy Technology Data Exchange (ETDEWEB)

    Ryan, T.P.; Dowdall, A.M.; Long, S.; Smith, V.; Pollard, D.; Cunningham, J.D. [Radiological Protection Institute of Ireland, 3 Clonskeagh Sq., Clonskeagh Rd., Dublin (Ireland)

    1999-08-01

    Plutonium and americium activity concentrations in fish and shellfish landed in Ireland in the period 1988 to 1997 are presented. Activity concentrations in fish are low and often below detection limits, while those in mussels and oysters sampled on the northeast coast show no significant signs of decline. The estimated doses to hypothetical typical and heavy seafood consumers remain below 1 {mu}Sv yr{sup -1} (committed effective dose).Plutonium activity concentrations measured in Fucus vesiculosus around the Irish coastline have not fallen appreciably in the ten year period between 1986 and 1996. Furthermore, the mean {sup 238}Pu/{sup 239,240}Pu ratio of 0.17{+-}0.05 in Fucus vesiculosus from the west coast of Ireland demonstrates the increasing significance of Sellafield-derived plutonium in those waters. (Copyright (c) 1999 Elsevier Science B.V., Amsterdam. All rights reserved.)

  14. Standard test method for determining plutonium by controlled-potential coulometry in H2SO4 at a platinum working electrode

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    1990-01-01

    1.1 This test method covers the determination of milligram quantities of plutonium in unirradiated uranium-plutonium mixed oxide having a U/Pu ratio range of 0.1 to 10. This test method is also applicable to plutonium metal, plutonium oxide, uranium-plutonium mixed carbide, various plutonium compounds including fluoride and chloride salts, and plutonium solutions. 1.2 The recommended amount of plutonium for each aliquant in the coulometric analysis is 5 to 10 mg. Precision worsens for lower amounts of plutonium, and elapsed time of electrolysis becomes impractical for higher amounts of plutonium. 1.3 The values stated in SI units are to be regarded as standard. No other units are to be regarded as standard. 1.4 This standard does not purport to address all of the safety concens, if any, associated with its use. It is the responsibility of the user of this standard to establish appropriate safety and health practices and determine the applicability of regulatory limitations prior to use. Specific precaution...

  15. Hydrogen yields from water on the surface of plutonium dioxide

    Energy Technology Data Exchange (ETDEWEB)

    Sims, Howard E., E-mail: howard.e.sims@nnl.co.uk [National Nuclear Laboratory, Harwell Science Park, Didcot, Oxon OX11 0QT (United Kingdom); Webb, Kevin J.; Brown, Jamie [National Nuclear Laboratory, Central Laboratory, Sellafield, Seascale CA20 1PG (United Kingdom); Morris, Darrell [Nuclear Decommissioning Authority, Herdus House, Westlakes Science and Technology Park, Moor Row, Cumbria CA24 3HU (United Kingdom); Taylor, Robin J., E-mail: robin.j.taylor@nnl.co.uk [National Nuclear Laboratory, Central Laboratory, Sellafield, Seascale CA20 1PG (United Kingdom)

    2013-06-15

    Highlights: ► Hydrogen evolution due to water radiolysis on samples of Sellafield PuO{sub 2}. ► Sharp increase in hydrogen evolution above 75% relative humidity. ► Hydrogen evolution due to radiolytic rather than thermal reaction. ► Analysis of trends from literature data. -- Abstract: The long term storage of separated plutonium dioxide (PuO{sub 2}) in sealed canisters requires an understanding of the processes occurring within the cans. This includes potential mechanisms that lead to can pressurisation, including the radiolysis of adsorbed water forming hydrogen. New measurements of H{sub 2} production rates from three sources of PuO{sub 2} show low rates at low water monolayer coverage but a sharp increase between 75% and 95% relative humidity. This behaviour being quite different to that reported for CeO{sub 2} and UO{sub 2}, which, therefore, cannot be considered as suitable analogues for PuO{sub 2}/H{sub 2}O radiation chemistry. It is concluded that surface recombination reactions are likely to be important in the radiation chemistry and that the H{sub 2} production arises from a radiolytic process and not a thermal reaction, at least in these experiments.

  16. Plutonium measurements by accelerator mass spectrometry at LLNL

    Energy Technology Data Exchange (ETDEWEB)

    McAninch, J E; Hamilton, T F; Broan, T A; Jokela, T A; Knezovich, T J; Ognibene, T J; Proctor, I D; Roberts, M L; Southon, J R; Vogel, J S; Sideras-Haddad, E

    1999-10-26

    Mass spectrometric methods provide sensitive, routine, and cost-effective analyses of long-lived radionuclides. Here the authors report on the status of work at Lawrence Livermore National Laboratory (LLNL) to develop a capability for actinide measurements by accelerator mass spectrometry (AMS) to take advantage of the high potential of AMS for rejection of interferences. This work demonstrates that the LLNL AMS spectrometer is well-suited for providing high sensitivity, robust, high throughput measurements of plutonium concentrations and isotope ratios. Present backgrounds are {approximately}2 x 10{sup 7}atoms per sample for environmental samples prepared using standard alpha spectrometry protocols. Recent measurements of {sup 239+240}Pu and {sup 241}Pu activities and {sup 240}Pu/{sup 239}Pu isotope ratios in IAEA reference materials agree well with IAEA reference values and with alpha spectrometry and recently published ICP-MS results. Ongoing upgrades of the AMS spectrometer are expected to reduce backgrounds below 1 x 10{sup 6} atoms per sample while allowing simplifications of the sample preparation chemistry. These simplifications will lead to lower per-sample costs, higher throughput, faster turn around and, ultimately, to larger and more robust data sets.

  17. Manufacturing of Plutonium Tensile Specimens

    Energy Technology Data Exchange (ETDEWEB)

    Knapp, Cameron M [Los Alamos National Laboratory

    2012-08-01

    Details workflow conducted to manufacture high density alpha Plutonium tensile specimens to support Los Alamos National Laboratory's science campaigns. Introduces topics including the metallurgical challenge of Plutonium and the use of high performance super-computing to drive design. Addresses the utilization of Abaqus finite element analysis, programmable computer numerical controlled (CNC) machining, as well as glove box ergonomics and safety in order to design a process that will yield high quality Plutonium tensile specimens.

  18. Conversion of Russian weapon-grade plutonium into oxide for mixed oxide (MOX) fuel fabrication

    Energy Technology Data Exchange (ETDEWEB)

    Glagovski, E.; Zakharkin, B. [A.A. Bochvar All-Russian Research Institute of Inorganic Materials, Russian Research Center, Moscow (Russian Federation); Kolotilov, Y. [Specialized State Design Institute, GSPI, Moscow (Russian Federation); Glagolenko, Y.; Skobtsov, A. [Mayak Production Association, Ozyorsk (Russian Federation); Zygmunt, S.; Mason, C.; Hahn, W.; Durrer, R. [Los Alamos National Lab., Nuclear Materials and Technology Div. NMT, Los Alamos, N.M. (United States); Thomas, S. [National Nuclear Security Administration, Washington DC (United States); Sicard, B.; Brossard, P.; Herlet, N. [CEA Marcoule 30 (France); Fraize, G.; Villa, A. [Cogema, 78 - Saint Quentin en Yvelines (France)

    2001-07-01

    Progress has been made in the Russian Federation towards the conversion of Russian weapons-grade plutonium (W-Pu) into plutonium oxide (PuO{sub 2}) suitable for further manufacture into mixed oxide (MOX) fuels. This program is funded both by French Commissariat at the Atomic Energy (CEA) and the US National Nuclear Security Administration (NNSA). The French program was started in the frame of the two cooperation agreements signed between Russian Federation and France in November 1992 concerning dismantling of nuclear weapons and the use of their nuclear materials for civilian purposes. The US program was started in 1998 in response to US proliferation concerns and the acknowledged international need to decrease available W-Pu. Russia has selected both the conversion process and the manufacturing site. This paper discusses the present state of development towards fulfilling this mission: the demonstration plant designed to process small amounts of Pu and validate all process stages and the industrial plant that will process up to 5 metric tons of Pu per year. (author)

  19. On the Burning of Plutonium Originating from Light Water Reactor Use in a Fast Molten Salt Reactor—A Neutron Physical Study

    OpenAIRE

    Bruno Merk; Dzianis Litskevich

    2015-01-01

    An efficient burning of the plutonium produced during light water reactor (LWR) operation has the potential to significantly improve the sustainability indices of LWR operations. The work offers a comparison of the efficiency of Pu burning in different reactor configurations—a molten salt fast reactor, a LWR with mixed oxide (MOX) fuel, and a sodium cooled fast reactor. The calculations are performed using the HELIOS 2 code. All results are evaluated against the plutonium burning efficiency d...

  20. Dismantlement and decontamination of a plutonium-238 facility at SRS

    Energy Technology Data Exchange (ETDEWEB)

    Smith, R.H. Jr.; Hootman, H.E.

    1994-01-01

    There has been very little, documented decontamination and decommissioning (D&D) experience on which to project cleanup costs and schedules for plutonium facilities at SRS and other DOE sites. A portion of the HB-Line, a plutonium-238 processing facility at SRS, has been undergoing D&D intermittently since 1984. Although this cleanup effort was not originally intended to quantify results, some key data have been project has demonstrated effective methods of accumulated, and the performing D&D work, and has demonstrated cleanup equipment and techniques under conditions of high contamination. Plutonium facilities where D&D is already underway provide an opportunity for` timely field testing of characterization, size reduction, and decontamination techniques. Some data are presented here; however, more specific tests and data may be obtained during the remainder of this project. This project has been recommended as a candidate test facility for a DOE planned ``Integrated D&D Demonstration`` managed by EM-50 to develop and demonstrate technology for D&D and surplus facilities deactivation. Both the remainder of this project and the Integrated D&D Demonstration Program can benefit from a joint effort, and the, overall costs should be reduced.

  1. Determination of plutonium isotopes in waters and environmental solids: A review

    DEFF Research Database (Denmark)

    Qiao, Jixin; Hou, Xiaolin; Miró, Manuel;

    2009-01-01

    accidents, and the discharge of nuclear waste. This article summarizes and critically compares recently reported methods for determination of Pu isotopes in waters and environmental solid substrates, in which sample pre-treatment is imperative for separation of the target species from matrix ingredients and......A number of analytical methods have been developed in the past few years for environmental monitoring of plutonium (Pu) isotopes around nuclear facilities within protocols for emergency preparedness as well as for risk assessment of contaminated areas resulting from nuclear weapon tests, nuclear...

  2. Plutonium and americium in arctic waters, the North Sea and Scottish and Irish coastal zones

    DEFF Research Database (Denmark)

    Hallstadius, L.; Aarkrog, Asker; Dahlgaard, Henning

    1986-01-01

    Plutonium and americium have been measured in surface waters of the Greenland and Barents Seas and in the northern North Sea from 1980 through 1984. Measurements in water and biota, Fucus, Mytilus and Patella, were carried out in North-English and Scottish waters in 1982 and Fucus samples were...... of the Irish Sea) to Spitsbergen. 241Am found in Arctic waters probably originates from the decay of fallout 241Pu and, like Pu, tentatively has a residence time of the order of several years. Americium from Sellafield has an estimated mean residence time of 4–6 months in Scottish waters....

  3. Designing Pu600 for Authentication

    Energy Technology Data Exchange (ETDEWEB)

    White, G

    2008-07-10

    Many recent Non-proliferation and Arms Control software projects include an authentication component. Demonstrating assurance that software and hardware performs as expected without hidden 'back-doors' is crucial to a project's success. In this context, 'authentication' is defined as determining that the system performs only its intended purpose and performs that purpose correctly and reliably over many years. Pu600 is a mature software solution for determining the presence of Pu and the ratio of Pu240 to Pu239 by analyzing the gamma ray spectra in the 600 KeV region. The project's goals are to explore hardware and software technologies which can by applied to Pu600 which ease the authentication of a complete, end-to-end solution. We will discuss alternatives and give the current status of our work.

  4. A multi-radionuclide approach to evaluate the suitability of (239+240)Pu as soil erosion tracer.

    Science.gov (United States)

    Meusburger, Katrin; Mabit, Lionel; Ketterer, Michael; Park, Ji-Hyung; Sandor, Tarjan; Porto, Paolo; Alewell, Christine

    2016-10-01

    Fallout radionuclides have been used successfully worldwide as tracers for soil erosion, but relatively few studies exploit the full potential of plutonium (Pu) isotopes. Hence, this study aims to explore the suitability of the plutonium isotopes (239)Pu and (240)Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as (137)Cs and (210)Pbex. As test area an erosion affected headwater catchment of the Lake Soyang (South Korea) was selected. All three fallout radionuclides confirmed high erosion rates for agricultural sites (>25tha(-1)yr(-1)). Pu isotopes further allowed determining the origin of the fallout. Both (240)Pu/(239)Pu atomic ratios and (239+240)Pu/(137)Cs activity ratios were close to the global fallout ratio. However, the depth profile of the (239+240)Pu/(137)Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of (239+240)Pu. The activity ratios further indicated preferential transport of (137)Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the (239+240)Pu/(137)Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both (137)Cs and (239+240)Pu have the same fallout source. Implementing this particle size correction factor in the conversion of (137)Cs inventories resulted in comparable estimates of soil loss for (137)Cs and (239+240)Pu. The comparison among the different fallout radionuclides highlights the suitability of (239+240)Pu through less preferential transport compared to (137)Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, (239+240)Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the soil and lateral transport during water erosion was shown to differ from that of (137)Cs, there is a clear

  5. Detection of long-lived plutonium isotopes in environmental samples by Accelerator Mass Spectrometry (AMS)

    Energy Technology Data Exchange (ETDEWEB)

    Hain, Karin; Faestermann, Thomas; Fimiani, Leticia; Gomez Guzman, Jose Manuel; Korschinek, Gunther; Ludwig, Peter [Technische Universitaet Muenchen (Germany); Shinonaga, Taeko [Helmholtz Zentrum Muenchen (Germany)

    2013-07-01

    The Plutonium isotopes {sup 239}Pu (T{sub 1/2}=2.4.10{sup 4}a), {sup 240}Pu (T{sub 1/2}=6.5.10{sup 3}a) and {sup 242}Pu (T{sub 1/2}=3.7.10{sup 5}a) are anthropogenic radionuclides emitted into the environment by nuclear activities. Pu is accumulated in the human body and hence, poses a considerable hazard to human health. Due to the long half-lives, these isotopes are present in the biosphere on large time scales and a build-up can be expected. Therefore it is important to study the contamination pathway of Pu into the drinking water. At the Maier-Leibnitz-Laboratory in Munich a method to detect long-lived Pu isotopes by Accelerator Mass Spectrometry (AMS) is being developed. AMS requires only few milligrams of sample material, which is a substantial advantage over decay counting techniques. Consequently, more samples from different locations can be taken which is essential when searching for locally increased Pu concentrations as in the Pacific Ocean after the Fukushima accident in March 2011. Samples from different locations in the Pacific Ocean and from the snow-hydrosphere are planned to be investigated by AMS. The principle detection method using AMS and an overview of the status of the project is presented.

  6. Solution speciation of plutonium and Americium at an Australian legacy radioactive waste disposal site.

    Science.gov (United States)

    Ikeda-Ohno, Atsushi; Harrison, Jennifer J; Thiruvoth, Sangeeth; Wilsher, Kerry; Wong, Henri K Y; Johansen, Mathew P; Waite, T David; Payne, Timothy E

    2014-09-01

    During the 1960s, radioactive waste containing small amounts of plutonium (Pu) and americium (Am) was disposed in shallow trenches at the Little Forest Burial Ground (LFBG), located near the southern suburbs of Sydney, Australia. Because of periodic saturation and overflowing of the former disposal trenches, Pu and Am have been transferred from the buried wastes into the surrounding surface soils. The presence of readily detected amounts of Pu and Am in the trench waters provides a unique opportunity to study their aqueous speciation under environmentally relevant conditions. This study aims to comprehensively investigate the chemical speciation of Pu and Am in the trench water by combining fluoride coprecipitation, solvent extraction, particle size fractionation, and thermochemical modeling. The predominant oxidation states of dissolved Pu and Am species were found to be Pu(IV) and Am(III), and large proportions of both actinides (Pu, 97.7%; Am, 86.8%) were associated with mobile colloids in the submicron size range. On the basis of this information, possible management options are assessed.

  7. Accumulation of plutonium in mammalian wildlife tissues following dispersal by accidental-release tests.

    Science.gov (United States)

    Johansen, M P; Child, D P; Caffrey, E A; Davis, E; Harrison, J J; Hotchkis, M A C; Payne, T E; Ikeda-Ohno, A; Thiruvoth, S; Twining, J R; Beresford, N A

    2016-01-01

    We examined the distribution of plutonium (Pu) in the tissues of mammalian wildlife inhabiting the relatively undisturbed, semi-arid former Taranaki weapons test site, Maralinga, Australia. The accumulation of absorbed Pu was highest in the skeleton (83% ± 6%), followed by muscle (10% ± 9%), liver (6% ± 6%), kidneys (0.6% ± 0.4%), and blood (0.2%). Pu activity concentrations in lung tissues were elevated relative to the body average. Foetal transfer was higher in the wildlife data than in previous laboratory studies. The amount of Pu in the gastrointestinal tract was highly elevated relative to that absorbed within the body, potentially increasing transfer of Pu to wildlife and human consumers that may ingest gastrointestinal tract organs. The Pu distribution in the Maralinga mammalian wildlife generally aligns with previous studies related to environmental exposure (e.g. Pu in humans from worldwide fallout), but contrasts with the partitioning models that have traditionally been used for human worker-protection purposes (approximately equal deposition in bone and liver) which appear to under-predict the skeletal accumulation in environmental exposure conditions.

  8. Standard test method for the determination of impurities in plutonium metal: acid digestion and inductively coupled plasma-mass spectroscopy (ICP-MS) analysis

    CERN Document Server

    American Society for Testing and Materials. Philadelphia

    2006-01-01

    1.1 This Test Method covers the determination of 58 trace elements in plutonium (Pu) metal. The Pu sample is dissolved in acid, and the concentration of the trace impurities are determined by Inductively Coupled Plasma-Mass Spectroscopy (ICP-MS). 1.2 This Test Method is specific for the determination of trace impurities in Pu metal. It may be applied to other types of Pu materials, such as Pu oxides, if the samples are dissolved and oxidized to the Pu(IV) state. However, it is the responsibility of the user to evaluate the performance of other matrices. 1.3 This standard does not purport to address all of the safety concerns associated with its use. It is the responsibility of the user of this method to establish appropriate safety and health practices and to determine the applicability of regulatory limitations prior to use of this standard.

  9. SOLUBILITY OF URANIUM AND PLUTONIUM IN ALKALINE SAVANNAH RIVER SITE HIGH LEVEL WASTE SOLUTIONS

    Energy Technology Data Exchange (ETDEWEB)

    King, W.; Hobbs, D.; Wilmarth, B.; Edwards, T.

    2010-03-10

    Five actual Savannah River Site tank waste samples and three chemically-modified samples were tested to determine solubility limits for uranium and plutonium over a one year time period. Observed final uranium concentrations ranged from 7 mg U/L to 4.5 g U/L. Final plutonium concentrations ranged from 4 {micro}g Pu/L to 12 mg Pu/L. Actinide carbonate complexation is believed to result in the dramatic solubility increases observed for one sample over long time periods. Clarkeite, NaUO{sub 2}(O)OH {center_dot} H{sub 2}O, was found to be the dominant uranium solid phase in equilibrium with the waste supernate in most cases.

  10. Determination of plutonium in environmental samples by controlled valence in anion exchange

    DEFF Research Database (Denmark)

    Chen, Q.J.; Aarkrog, A.; Nielsen, S.P.

    1993-01-01

    is heated at 400-degrees-C and digested in aqua regia. Na2SO3 and NaNO2 have been applied to obtain the Pu4+ valence state in 0.571 N HN03 for different samples. Plutonium and thorium are coadsorbed on anionic resin from 8N HN03. The column is eluted with 8N HN03 containing fresh NaNO2 to keep the Pu4......+ state for uranium decontamination. The system of the column is changed from 8N HNO3 to concentrated HCl with 50 ml concentrated HCI containing a few milligrams of NaNO2. Further decontamination of thorium was achieved by elution with concentrated HCI instead of 9N HCl. The plutonium is successfully...

  11. Rapid and automated determination of plutonium and neptunium in environmental samples

    Energy Technology Data Exchange (ETDEWEB)

    Qiao, J.

    2011-03-15

    This thesis presents improved analytical methods for rapid and automated determination of plutonium and neptunium in environmental samples using sequential injection (SI) based chromatography and inductively coupled plasma mass spectrometry (ICP-MS). The progress of methodology development in this work consists of 5 subjects stated as follows: 1) Development and optimization of an SI-anion exchange chromatographic method for rapid determination of plutonium in environmental samples in combination of inductively coupled plasma mass spectrometry detection (Paper II); (2) Methodology development and optimization for rapid determination of plutonium in environmental samples using SI-extraction chromatography prior to inductively coupled plasma mass spectrometry (Paper III); (3) Development of an SI-chromatographic method for simultaneous determination of plutonium and neptunium in environmental samples (Paper IV); (4) Investigation of the suitability and applicability of 242Pu as a tracer for rapid neptunium determination using anion exchange chromatography in an SI-network coupled with inductively coupled plasma mass spectrometry (Paper V); (5) Exploration of macro-porous anion exchange chromatography for rapid and simultaneous determination of plutonium and neptunium within an SI system (Paper VI). The results demonstrate that the developed methods in this study are reliable and efficient for accurate assays of trace levels of plutonium and neptunium as demanded in different situations including environmental risk monitoring and assessment, emergency preparedness and surveillance of contaminated areas. (Author)

  12. A proteomic approach to identification of plutonium-binding proteins in mammalian cells.

    Science.gov (United States)

    Aryal, Baikuntha P; Paunesku, Tatjana; Woloschak, Gayle E; He, Chuan; Jensen, Mark P

    2012-02-16

    Plutonium can enter the body through different routes and remains there for decades; however its specific biochemical interactions are poorly defined. We, for the first time, have studied plutonium-binding proteins using a metalloproteomic approach with rat PC12 cells. A combination of immobilized metal ion chromatography, 2D gel electrophoresis, and mass spectrometry was employed to analyze potential plutonium-binding proteins. Our results show that several proteins from PC12 cells show affinity towards Pu(4+)-NTA (plutonium bound to nitrilotriacetic acid). Proteins from seven different spots in the 2D gel were identified. In contrast to the previously known plutonium-binding proteins transferrin and ferritin, which bind ferric ions, most identified proteins in our experiment are known to bind calcium, magnesium, or divalent transition metal ions. The identified plutonium interacting proteins also have functional roles in downregulation of apoptosis and other pro-proliferative processes. MetaCore™ analysis based on this group of proteins produced a pathway with a statistically significant association with development of neoplastic diseases.

  13. Verification of plutonium content in spent fuel assemblies using neutron self-interrogation

    Energy Technology Data Exchange (ETDEWEB)

    Menlove, Howard O [Los Alamos National Laboratory; Menlove, Apencer H [Los Alamos National Laboratory; Tobin, Stephen J [Los Alamos National Laboratory

    2009-01-01

    The large amounts of plutonium in reactor spent fuel assemblies has led to increased research directed toward the measurement of the plutonium for safeguards verification. The high levels of fission product gamma-ray activity and curium neutron backgrounds have made the plutonium measurement difficult. We have developed a new technique that can directly measure both the {sup 235}U concentration and the plutonium fissile concentration using the intrinsic neutron emission fronl the curium in the fuel assembly. The passive neutron albedo reactivity (PNAR) method has been described previously where the curium neutrons are moderated in the surrounding water and reflect back into the fuel assembly to induce fissions in the fissile material in the assembly. The cadmium (Cd) ratio is used to separate the spontaneous fission source neutrons from the reflected thermal neutron fission reactions. This method can measure the sum of the {sup 235}U and the plutonium fissile mass, but not the separate components. Our new differential die-away self-interrogation method (DDSI) can be used to separate the {sup 235}U from the {sup 239}Pu. The method has been applied to both fuel rods and full assemblies. For fuel rods the epi-thermal neutron reflection method filters the reflected neutrons through thin Cd filters so that the reflected neutrons are from the epi-cadmium energy region. The neutron fission energy response in the epi-cadmium region is distinctly different for {sup 235}U and {sup 239}Pu. We are able to measure the difference between {sup 235}U and {sup 239}Pu by sampling the neutron induced fission rate as a function of time and multiplicity after the initial fission neutron is detected. We measure the neutron fission rate using list-mode data collection that stores the time correlations between all of the counts. The computer software can select from the data base the time correlations that include singles, doubles, and triples. The die-away time for the doubles

  14. Treatment of plutonium process residues by molten salt oxidation

    Energy Technology Data Exchange (ETDEWEB)

    Stimmel, J.; Wishau, R.; Ramsey, K.B.; Montoya, A.; Brock, J. [Los Alamos National Lab., NM (United States); Heslop, M. [Naval Surface Warfare Center (United States). Indian Head Div.; Wernly, K. [Molten Salt Oxidation Corp. (United States)

    1999-04-01

    Molten Salt Oxidation (MSO) is a thermal process that can remove more than 99.999% of the organic matrix from combustible {sup 238}Pu material. Plutonium processing residues are injected into a molten salt bed with an excess of air. The salt (sodium carbonate) functions as a catalyst for the conversion of the organic material to carbon dioxide and water. Reactive species such as fluorine, chlorine, bromine, iodine, sulfur, phosphorous and arsenic in the organic waste react with the molten salt to form the corresponding neutralized salts, NaF, NaCl, NaBr, NaI, Na{sub 2}SO{sub 4}, Na{sub 3}PO{sub 4} and NaAsO{sub 2} or Na{sub 3}AsO4. Plutonium and other metals react with the molten salt and air to form metal salts or oxides. Saturated salt will be recycled and aqueous chemical separation will be used to recover the {sup 238}Pu. The Los Alamos National Laboratory system, which is currently in the conceptual design stage, will be scaled down from current systems for use inside a glovebox.

  15. Estimation of 240Pu Mass in a Waste Tank Using Ultra-Sensitive Detection of Radioactive Xenon Isotopes from Spontaneous Fission

    Energy Technology Data Exchange (ETDEWEB)

    Bowyer, Ted W. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Gesh, Christopher J. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Haas, Derek A. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Hayes, James C. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Mahoney, Lenna A. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Meacham, Joseph E. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Mendoza, Donaldo P. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Olsen, Khris B. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Prinke, Amanda M. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Reid, Bruce D. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Woods, Vincent T. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2014-12-01

    We report on a technique to detect and quantify the amount of 240Pu in a large tank used to store nuclear waste from plutonium production at the Hanford nuclear site. While the contents of this waste tank are known from previous grab sample measurements, our technique could allow for determination of the amount of 240Pu in the tank without costly sample retrieval and analysis of this highly radioactive material. This technique makes an assumption, which was confirmed, that 240Pu dominates the spontaneous fissions occurring in the tank.

  16. Safety analysis report for the /sup 238/PuO/sub 2/ fuel form facility

    Energy Technology Data Exchange (ETDEWEB)

    Angerman, C.L.; Bickford, D.F.; Gould, T.H. Jr.; Smith, P.K.

    1977-08-01

    The Plutonium Fuel Form (PuFF) Facility has been constructed at the Savannah River Plant to manufacture 30 to 60 kg/yr of /sup 238/Pu fuel forms for space power applications. This facility is located in the existing Building 235-F near the geographical center of the Savannah River Plant (SRP) site. Pilot production is scheduled to begin in July 1977, with full-scale production in April 1978. The process line of the facility consists of nine separate, interconnected shielded cells; five shielded wing cabinets or glove boxes; three hoods; and contained auxiliary equipment. These process enclosures will be, for the most part, under an atmosphere of recirculating inert gas. The products of the facility will be dense fuel forms manufactured from PuO/sub 2/ powder with a nominal isotopic composition of 80% /sup 238/Pu-20% /sup 239/Pu. This powder, made from calcined oxalate, has been produced safely at a rate of about 20 kg /sup 238/Pu/yr in the H-Area B-Line in Building 221-H for approximately ten years. This report describes design objectives, nature of operations, potential hazards and limiting factors, facility response to postulated accidents and failures, and environmental effects. The results of the analyses described in this report indicate that the facility has the capacity to prevent or sufficiently reduce accidents that represent potential risks to health and safety. The safety analysis in conjunction with process requirements provides the bases for Technical Standards for operation. The analysis also documents the degree of conformance of the facility design with the General Design Criteria - Plutonium Facilities and the Environmental Statement.

  17. Rapid and Automated Determination of Plutonium and Neptunium in Environmental Samples

    DEFF Research Database (Denmark)

    Qiao, Jixin

    and optimization for rapid determination of plutonium in environmental samples using SIextraction chromatography prior to inductively coupled plasma mass spectrometry (Paper III); (3) Development of an SI-chromatographic method for simultaneous determination of plutonium and neptunium in environmental samples...... (Paper IV); (4) Investigation of the suitability and applicability of 242Pu as a tracer for rapid neptunium determination using anion exchange chromatography in an SI-network coupled with inductively coupled plasma mass spectrometry (Paper V); (5) Exploration of macro-porous anion exchange chromatography......This thesis presents improved analytical methods for rapid and automated determination of plutonium and neptunium in environmental samples using sequential injection (SI) based chromatography and inductively coupled plasma mass spectrometry (ICP-MS). The progress of methodology development...

  18. Development of the DGT technique for in-situ Pu speciation measurements

    Energy Technology Data Exchange (ETDEWEB)

    Cusnir, R.; Bochud, F.; Froidevaux, P. [Institute of Radiation Physics, Lausanne University Hospital, Rue du Grand-Pre 1, CH-1007 Lausanne (Switzerland); Steinmann, P. [Federal Office of Public Health, Swarzenburgstrasse 165, CH-3003 Bern (Switzerland)

    2014-07-01

    Toxic effects of artificial radionuclides are strongly dependent on the surrounding chemical environment which determines the bioavailability of contaminant species. Speciation of plutonium in the environment is of particular interest since it is a long-life actinide contributing to the dose exposure via ingestion with water and food in case of radioactive discharge. Furthermore, natural colloids present in waters, as main carriers of dissolved trace metals, can transport plutonium over significant distances from contaminated sites. The diffusive gradients in thin films (DGT) technique is an efficient instrument for passive sampling of trace metals. It allows for in-situ monitoring of mean concentrations of bioavailable contaminant species (1). A DGT sampler consists of two gel layers: a polyacrylamide hydrogel diffusion layer allowing to diffuse labile metal species to the second, binding layer, impregnated with ion-exchange resin. Resin elution and further analysis allow determining the amount of the bioavailable fraction of trace metals in the bulk solution, which can be calculated from the relationship: C{sub bulk}= (M x Δg)/(D x t x A) where M is the measured metal species inventory in the resin, Δg the thickness of the diffusion layer, D the diffusion coefficient of the species in the gel, t the time of deployment, A the diffusion area. To our knowledge, the DGT has not yet been applied for Pu speciation measurements and the D value is unknown. Here we propose the use of DGT to monitor the dissolved phase and labile complexes of plutonium in the aquatic environment. We have first measured the diffusion coefficient of plutonium in the hydrogel. Experiments were carried out in a diffusion cell (2) and with commercially available DGT samplers exposed in standardized solutions containing {sup 239}Pu at pico-molar concentrations. Both approaches give comparable D values in the range of 2.30 x 10{sup -6} - 2.45 x 10{sup -6} cm{sup 2} s{sup -1}. We then studied

  19. Plutonium and Uranium Atom Ratios and Activity Levels in Cochiti Lake Bottom Sediments Provided by Pueblo de Cochiti

    Energy Technology Data Exchange (ETDEWEB)

    Gallaher, B.M.; Efurd, D.W.; Rokop, D.J.; Benjamin, T.M.

    1999-05-01

    Historical operations at the Los Alamos National Laboratory have contaminated stream sediments with plutonium and other radionuclides. A small portion of these contaminated sediments has been carried by floods into the Rio Grande drainage system, eventually to be trapped by Cochiti Lake located on Pueblo de Cochiti lands approximately 8 km downstream of the Laboratory. In this study, lake bottom sediment samples provided by the Pueblo de Cochiti were analyzed by thermal ionization mass spectrometry to determine plutonium and uranium activity levels and isotopic atom ratios. This specialized analytical method allows us to take isotopic fingerprints of radionuclides found in the sediment and to determine how much plutonium and uranium came from the Laboratory and how much was deposited by worldwide fallout or is natural. Two distinct types of samples were processed: segments of a continuous vertical core of the entire accumulated sediment sequence and other samples from across the lake bottom at the water/sediment interface. Based on measurement of the {sup 240}Pu/{sup 239}Pu atom ratio, Laboratory-derived plutonium is present in eight of nine samples at the core site. On a depth-weighted basis, approximately one-half of the {sup 239}Pu and {sup 240}Pu came from early operations at the Laboratory; the remaining plutonium came from fallout dispersed by above-ground nuclear tests. In contrast to the core site, the samples from the other locations showed little or no evidence of Laboratory-derived plutonium, with more than 90 percent of the plutonium attributable to fallout. The overall amount of plutonium in all the samples is of the same magnitude as other reservoirs in the region. The net increase in plutonium over upstream reservoirs unaffected by Laboratory activities is a maximum of 0.014 pCi/g or 3.5 times. All of the samples reflect natural uranium compositions. Laboratory-derived uranium is not identifiable, presumably because the sediment contains abundant

  20. 计算机模拟研究Pu4+在人体血浆中的分布%Computer simulation of Pu(Ⅳ) speciation in human blood plasma

    Institute of Scientific and Technical Information of China (English)

    邓冰; 蒋树斌; 董兰; 董亮

    2014-01-01

    A thermodynamic equilibrium models consisted of multi-metal ion and low molecular-weight ligands has been constructed to study the speciation of Pu4+ in human blood plasma and the influences of total concentration of DTPA、CO3 2-and Citrate3- on the speciation. Computer simulation indicated that low concentration of plutonium in plasma fluid with Pu(OH)4(aq)species accumula-ted in liver. Pu4+ form precipitation is difficult to eliminate from the body under the high concentration of plutonium in plasma flu-ids. At the concentrations of DTPA was 2. 5 × 10-5 mol·L-1 , the species of plutonium mainly as negatively charged [ Pu ( OH ) DT-PA]2- and maintain stable. The speciation was at first calculated at pH 5. 0,with the increase of concentration of[Citrate3-],the major species of Pu4+ as[ PuCitrate2 ] 2-and[ PuCitrate]+ which were excreted easily from body. In blood plasma Pu4+ combined with Ca2+、Mg2+ to form[CaHDTPA]2-、[Ca2DTPA]-、[CaDTPA]3-、[MgHDTPA]2-、[MgDTPA]3- when[DTPA]at 4.6×10-5mol· L-1 ,which excrete Pu(Ⅳ) and produce toxic side effects on bone at the same time.%建立了由多种金属离子和小分子配体组成的多相人体血浆热力学平衡模型。模拟研究了Pu4+在血浆的形态分布及二乙三胺五乙酸( DTPA)和CO32-、Citrate3-浓度对细胞液中Pu4+形态分布的影响。血浆中的低浓度Pu(Ⅳ)易以Pu(OH)4(aq)的形态蓄积在肝脏中,钚浓度升高则形成沉淀Pu(OH)4(s)难以排出。在[DTPA]=2.5×10-5mol·L-1时,血浆中水溶性小分子[Pu(OH)DTPA]2-含量达到最高并保持稳定。酸性条件下随着[ Citrate3-]的升高,血浆中Pu4+与Citrate3-结合形成可溶性的[ PuCitrate2]2-和[ PuCitrate]+离子化合物。[DTPA]>4.6×10-5mol·L-1时,血浆中的 DTPA以与 Ca2+、Mg2+结合的[CaHDTPA]2-、[Ca2DTPA]-、[CaDT-PA]3-、[ MgHDTPA]2-、[ MgDTPA]3-小分子结合态为主。

  1. Sequential injection approach for simultaneous determination of ultratrace plutonium and neptunium in urine with accelerator mass spectrometry.

    Science.gov (United States)

    Qiao, Jixin; Hou, Xiaolin; Roos, Per; Lachner, Johannes; Christl, Marcus; Xu, Yihong

    2013-09-17

    An analytical method was developed for simultaneous determination of ultratrace level plutonium (Pu) and neptunium (Np) using iron hydroxide coprecipitation in combination with automated sequential injection extraction chromatography separation and accelerator mass spectrometry (AMS) measurement. Several experimental parameters affecting the analytical performance were investigated and compared including sample preboiling operation, aging time, amount of coprecipitating reagent, reagent for pH adjustment, sedimentation time, and organic matter decomposition approach. The overall analytical results show that preboiling and aging are important for obtaining high chemical yields for both Pu and Np, which is possibly related to the aggregation and adsorption behavior of organic substances contained in urine. Although the optimal condition for Np and Pu simultaneous determination requires 5-day aging time, an immediate coprecipitation without preboiling and aging could also provide fairly satisfactory chemical yields for both Np and Pu (50-60%) with high sample throughput (4 h/sample). Within the developed method, (242)Pu was exploited as chemical yield tracer for both Pu and Np isotopes. (242)Pu was also used as a spike in the AMS measurement for quantification of (239)Pu and (237)Np concentrations. The results show that, under the optimal experimental condition, the chemical yields of (237)Np and (242)Pu are nearly identical, indicating the high feasibility of (242)Pu as a nonisotopic tracer for (237)Np determination in real urine samples. The analytical method was validated by analysis of a number of urine samples spiked with different levels of (237)Np and (239)Pu. The measured values of (237)Np and (239)Pu by AMS exhibit good agreement (R(2) ≥ 0.955) with the spiked ones confirming the reliability of the proposed method.

  2. Laboratory and field studies of polonium and plutonium in marine plankton

    Energy Technology Data Exchange (ETDEWEB)

    Wilson, R.C. [Westlakes Scientific Consulting Ltd., Princess Royal Building, Westlakes Science and Technology Park, Moor Row, Cumbria CA24 3LN (United Kingdom)], E-mail: richard.c.wilson@westlakes.ac.uk; Watts, S.J.; Vives i Batlle, J.; McDonald, P. [Westlakes Scientific Consulting Ltd., Princess Royal Building, Westlakes Science and Technology Park, Moor Row, Cumbria CA24 3LN (United Kingdom)

    2009-08-15

    Uptake experiments were successfully undertaken for polonium and plutonium in the marine diatom Skeletonema costatum. Experiments were complemented with a field study which yielded concentration factors for these radionuclides for plankton samples collected in the eastern Irish Sea. The uptake experiment produced uptake half times of 0.8 and 0.6 days for plutonium and polonium, respectively. Concentration factors of 3.1 x 10{sup 5} l kg{sup -1} for plutonium and 2.4 x 10{sup 5} l kg{sup -1} for polonium were consistent with those suggested by the IAEA for phytoplankton. Concentration factors derived from the field study were 2 x 10{sup 3} l kg{sup -1} for plutonium and 1.4 x 10{sup 4} l kg{sup -1} for polonium and were more consistent with IAEA values for zooplankton rather than phytoplankton. The maximum calculated dose rate due to Po and Pu in plankton sampled in the field was 0.12 {mu}Gy h{sup -1}. In applying the laboratory-derived phytoplankton CF values for Po and Pu, higher dose rates, in the range 6-11 {mu}Gy h{sup -1}, were calculated. The latter values are well below the UNSCEAR and IAEA review value of 400 {mu}Gy h{sup -1}, and are also below the Environment Agency marine action level of 40 {mu}Gy h{sup -1}.

  3. Plutonium contamination in soils in open space and residential areas near Rocky Flats, Colorado.

    Science.gov (United States)

    Litaor, M I

    1999-02-01

    Spatial analysis of the 240Pu:239Pu isotopic ratio of 42 soil samples collected around Rocky Flats Plant near Golden, Colorado, was conducted to assess the effect of Rocky Flats Plant activity on the soil environment. Two probability maps that quantified the uncertainty of the spatial distribution of plutonium isotopic ratios were constructed using the sequential Gaussian simulation technique (sGs). Assuming a plutonium isotopic ratio range of 0.152+/-0.003 to 0.169+/-0.009 is characteristic to global fallout in Colorado, and a mean value of 0.155 is representative for the Rocky Flats Plant area, the main findings of the current work were (1) the areas northwest and southwest of Rocky Flats Plant exhibited a plutonium ratio > or = 0.155, thus were minimally impacted by the plant activity; (2) the study area east of Rocky Flats Plant (approximately 120 km2) exhibited a plutonium isotopic ratio open space and residential areas amounted to 111.2 GBq, with a standard error of estimate of 50.8 GBq.

  4. Laboratory and field studies of polonium and plutonium in marine plankton.

    Science.gov (United States)

    Wilson, R C; Watts, S J; Vives i Batlle, J; McDonald, P

    2009-08-01

    Uptake experiments were successfully undertaken for polonium and plutonium in the marine diatom Skeletonema costatum. Experiments were complemented with a field study which yielded concentration factors for these radionuclides for plankton samples collected in the eastern Irish Sea. The uptake experiment produced uptake half times of 0.8 and 0.6 days for plutonium and polonium, respectively. Concentration factors of 3.1 x 10(5) l kg(-1) for plutonium and 2.4 x 10(5) l kg(-1) for polonium were consistent with those suggested by the IAEA for phytoplankton. Concentration factors derived from the field study were 2 x 10(3) l kg(-1) for plutonium and 1.4 x 10(4) l kg(-1) for polonium and were more consistent with IAEA values for zooplankton rather than phytoplankton. The maximum calculated dose rate due to Po and Pu in plankton sampled in the field was 0.12 microGyh(-1). In applying the laboratory-derived phytoplankton CF values for Po and Pu, higher dose rates, in the range 6-11 microGyh(-1), were calculated. The latter values are well below the UNSCEAR and IAEA review value of 400 microGyh(-1), and are also below the Environment Agency marine action level of 40 microGyh(-1).

  5. Assessment of the risk of transporting plutonium dioxide by cargo aircraft

    Energy Technology Data Exchange (ETDEWEB)

    McSweeney, T.I.; Johnson, J.F.

    1977-06-01

    To enable easy comparison, all the plutonium shipping evaluations have used the same bases. In each, the results have been related to a future time--the early 1980s--when plutonium shipments are expected to be more frequent. The characteristics of the nuclear economy used in this analysis are: A total of 18 metric tons (MT) of plutonium is shipped annually, via the mode being evaluated. 100 kg of plutonium are transported per shipment. For air shipment, a truck and air segment are considered. The average shipping distance per shipment is 1,422 miles with 14 percent of the distance being by truck. Shipping systems and regulations are the same as in 1974. PuO/sub 2/ is shipped in 6M containers. The use of other shipping conditions could result in different risks than reported here. For the purposes of this study, plutonium dioxide was assumed to be carried exclusively in the 15-gal version of the 6M container. Unless otherwise noted, all references to 6M containers in the report refer to this particular size. Based on the shipping assumptions, the likelihood that an aircraft carrying a shipment will be involved in an accident is estimated to be about once in 450 years. For the projected shipping rate in the early 1980s, the likelihood of a release of plutonium as a result of shipment by air is one in 900 years for dioxide powder in the 6M container. The comparison of the truck and air transport modes for the same material showed truck transport to have less risk. At the same time, the air transport of plutonium dioxide was demonstrated to have a lower risk than other commonly accepted societal risks. The major contributor to the overall risk spectra for air transport was a cargo airplane, carrying plutonium dioxide, crashing at high speed into hard rock.

  6. Preconceptual design for separation of plutonium and gallium by ion exchange

    Energy Technology Data Exchange (ETDEWEB)

    DeMuth, S.F.

    1997-09-30

    The disposition of plutonium from decommissioned nuclear weapons, by incorporation into commercial UO{sub 2}-based nuclear reactor fuel, is a viable means to reduce the potential for theft of excess plutonium. This fuel, which would be a combination of plutonium oxide and uranium oxide, is referred to as a mixed oxide (MOX). Following power generation in commercial reactors with this fuel, the remaining plutonium would become mixed with highly radioactive fission products in a spent fuel assembly. The radioactivity, complex chemical composition, and large size of this spent fuel assembly, would make theft difficult with elaborate chemical processing required for plutonium recovery. In fabricating the MOX fuel, it is important to maintain current commercial fuel purity specifications. While impurities from the weapons plutonium may or may not have a detrimental affect on the fuel fabrication or fuel/cladding performance, certifying the effect as insignificant could be more costly than purification. Two primary concerns have been raised with regard to the gallium impurity: (1) gallium vaporization during fuel sintering may adversely affect the MOX fuel fabrication process, and (2) gallium vaporization during reactor operation may adversely affect the fuel cladding performance. Consequently, processes for the separation of plutonium from gallium are currently being developed and/or designed. In particular, two separation processes are being considered: (1) a developmental, potentially lower cost and lower waste, thermal vaporization process following PuO{sub 2} powder preparation, and (2) an off-the-shelf, potentially higher cost and higher waste, aqueous-based ion exchange (IX) process. While it is planned to use the thermal vaporization process should its development prove successful, IX has been recommended as a backup process. This report presents a preconceptual design with material balances for separation of plutonium from gallium by IX.

  7. Destruction of plutonium using non-uranium fuels in pressurized water reactor peripheral assemblies

    Energy Technology Data Exchange (ETDEWEB)

    Chodak, III, Paul [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

    1996-05-01

    This thesis examines and confirms the feasibility of using non-uranium fuel in a pressurized water reactor (PWR) radial blanket to eliminate plutonium of both weapons and civilian origin. In the equilibrium cycle, the periphery of the PWR is loaded with alternating fresh and once burned non-uranium fuel assemblies, with the interior of the core comprised of conventional three batch UO2 assemblies. Plutonium throughput is such that there is no net plutonium production: production in the interior is offset by destruction in the periphery. Using this approach a 50 MT WGPu inventory could be eliminated in approximately 400 reactor years of operation. Assuming all other existing constraints were removed, the 72 operating US PWRs could disposition 50 MT of WGPu in 5.6 years. Use of a low fissile loading plutonium-erbium inert-oxide-matrix composition in the peripheral assemblies essentially destroys 100% of the 239Pu and ≥90% {sub total}Pu over two 18 month fuel cycles. Core radial power peaking, reactivity vs EFPD profiles and core average reactivity coefficients were found to be comparable to standard PWR values. Hence, minimal impact on reload licensing is anticipated. Examination of potential candidate fuel matrices based on the existing experience base and thermo-physical properties resulted in the recommendation of three inert fuel matrix compositions for further study: zirconia, alumina and TRISO particle fuels. Objective metrics for quantifying the inherent proliferation resistance of plutonium host waste and fuel forms are proposed and were applied to compare the proposed spent WGPu non-uranium fuel to spent WGPu MOX fuels and WGPu borosilicate glass logs. The elimination disposition option spent non-uranium fuel product was found to present significantly greater barriers to proliferation than other plutonium disposal products.

  8. Destruction of plutonium using non-uranium fuels in pressurized water reactor peripheral assemblies

    Energy Technology Data Exchange (ETDEWEB)

    Chodak, P. III

    1996-05-01

    This thesis examines and confirms the feasibility of using non-uranium fuel in a pressurized water reactor (PWR) radial blanket to eliminate plutonium of both weapons and civilian origin. In the equilibrium cycle, the periphery of the PWR is loaded with alternating fresh and once burned non-uranium fuel assemblies, with the interior of the core comprised of conventional three batch UO{sub 2} assemblies. Plutonium throughput is such that there is no net plutonium production: production in the interior is offset by destruction in the periphery. Using this approach a 50 MT WGPu inventory could be eliminated in approximately 400 reactor years of operation. Assuming all other existing constraints were removed, the 72 operating US PWRs could disposition 50 MT of WGPu in 5.6 years. Use of a low fissile loading plutonium-erbium inert-oxide-matrix composition in the peripheral assemblies essentially destroys 100% of the {sup 239}Pu and {ge}90% {sub total}Pu over two 18 month fuel cycles. Core radial power peaking, reactivity vs EFPD profiles and core average reactivity coefficients were found to be comparable to standard PWR values. Hence, minimal impact on reload licensing is anticipated. Examination of potential candidate fuel matrices based on the existing experience base and thermo-physical properties resulted in the recommendation of three inert fuel matrix compositions for further study: zirconia, alumina and TRISO particle fuels. Objective metrics for quantifying the inherent proliferation resistance of plutonium host waste and fuel forms are proposed and were applied to compare the proposed spent WGPu non-uranium fuel to spent WGPu MOX fuels and WGPu borosilicate glass logs. The elimination disposition option spent non-uranium fuel product was found to present significantly greater barriers to proliferation than other plutonium disposal products.

  9. Effects of duration of fast and animal age on the gastrointestinal absorption of plutonium

    Energy Technology Data Exchange (ETDEWEB)

    Bhattacharyya, M.H.; Larsen, R.P.; Oldham, R.D.; Moretti, E.S.; Spaletto, M.I.

    1986-07-01

    The fraction of plutonium absorbed after oral administration of Pu(VI) to 24-h-fasted mice was 19 X 10(-4), 13-fold higher than in fed mice, 1.4 X 10(-4). We have investigated the relevance of the high gastrointestinal (GI) absorption value for the 24-h-fasted animals in setting drinking water standards for humans. When fasting was initiated at the beginning of the active phase of the mouse's daily activity cycle (when they would normally eat), plutonium GI absorption rose from 2.8 X 10(-4) at zero-time to a level typical of the 24-h-fasted mouse after only 2 h of fasting. In contrast, in mice allowed to eat for 4 h into their active phase prior to initiation of the fast (meal-fed mice), 8 h of fasting were required before GI absorption rose to a level similar to that of the 24-h-fasted mouse. The fraction of plutonium retained after gavage administration of Pu(VI) to 1-day-old rats was 74 X 10(-4), 70-fold higher than the value for fed adults. Retention after GI absorption in neonates remained 30- to 70-fold higher than in adults until weaning. One week after weaning, the fraction absorbed and retained by fed weanling rats was the same as that for fed adults, 1 X 10(-4). Drinking water standards for plutonium have been set based on GI absorption values for fed adult animals. The 10- to 100-fold increases in plutonium absorption in young and fasted animals reported by ourselves and others, and the rapid rise to fasted levels of absorption at the start of the animal's active phase, indicate that consideration should be given to elevated levels of plutonium absorption in young and fasted individuals.

  10. Plutonium behavior after pulmonary administration according to solubility properties, and consequences on alveolar macrophage activation.

    Science.gov (United States)

    Van der Meeren, Anne; Gremy, Olivier; Renault, Daniel; Miroux, Amandine; Bruel, Sylvie; Griffiths, Nina; Tourdes, Françoise

    2012-01-01

    The physico-chemical form in which plutonium enters the body influences the lung distribution and the transfer rate from lungs to blood. In the present study, we evaluated the early lung damage and macrophage activation after pulmonary contamination of plutonium of various preparation modes which produce different solubility and distribution patterns. Whatever the solubility properties of the contaminant, macrophages represent a major retention compartment in lungs, with 42 to 67% of the activity from broncho-alveolar lavages being associated with macrophages 14 days post-contamination. Lung changes were observed 2 and 6 weeks post-contamination, showing inflammatory lesions and accumulation of activated macrophages (CD68 positive) in plutonium-contaminated rats, although no increased proliferation of pneumocytes II (TTF-1 positive cells) was found. In addition, acid phosphatase activity in macrophages from contaminated rats was enhanced 2 weeks post-contamination as compared to sham groups, as well as inflammatory mediator levels (TNF-α, MCP-1, MIP-2 and CINC-1) in macrophage culture supernatants. Correlating with the decrease in activity remaining in macrophages after plutonium contamination, inflammatory mediator production returned to basal levels 6 weeks post-exposure. The production of chemokines by macrophages was evaluated after contamination with Pu of increasing solubility. No correlation was found between the solubility properties of Pu and the activation level of macrophages. In summary, our data indicate that, despite the higher solubility of plutonium citrate or nitrate as compared to preformed colloids or oxides, macrophages remain the main lung target after plutonium contamination and may participate in the early pulmonary damage.

  11. Carcinogenesis From Inhaled (PuO2)-Pu-239 in Beagles: Evidence for Radiation Homeostasis at Low Doses?

    Energy Technology Data Exchange (ETDEWEB)

    Fisher, Darrell R.; Weller, Richard E.

    2010-09-01

    From the early 1970s to the late 1980s, Pacific Northwest National Laboratory conducted life-span studies in beagle dogs on the biological effects of inhaled plutonium (239PuO2, 238PuO2, and 239Pu[NO3]4) to help predict risks associated with accidental intakes in workers. Years later, the purpose of the present follow-up study is to reassess the dose-response relationship for lung cancer induction in the 239PuO2 dogs compared to controls, with particular focus on the dose-response at low lung doses. A 239PuO2 aerosol (2.3 μm AMAD, 1.9 μm GSD) was administered to six groups of 20 young (18-month old) beagle dogs (10 males and 10 females) by inhalation at six different activity levels, as previously described in Laboratory reports. Control dogs were sham-exposed. In dose level 1, initial pulmonary lung depositions were 130 ± 48 Bq (3.5 ± 1.3 nCi), corresponding to 1 Bq g-1 lung tissue (0.029 ± 0.001 nCi g-1. Groups 2 through 6 received initial lung depositions (mean values) of 760, 2724, 10345, 37900, and 200000 Bq (22, 79, 300, 1100, and 5800 nCi) 239PuO2, respectively. For each dog, the absorbed dose to lungs was calculated from the initial lung burden and the final lung burden at time of death and lung mass, assuming a single, long-term retention function. Insoluble plutonium oxide exhibited long retention times in the lungs. Increased dose-dependent mortality due to lung cancer (bronchiolar-alveolar carcinoma, adenocarcinoma, epidermoid carcinoma) and radiation pneumonitis (highest exposures group) was observed in dogs exposed to 239PuO2. Calculated lung doses ranged from a few cGy in early-sacrificed dogs to 7764 cGy in dogs that experienced early deaths from radiation pneumonitis. Data were regrouped by lifetime lung dose and plotted as a function of lung tumor incidence. Lung tumor incidence in controls and zero-dose exposed dogs was 18% (5/28). However, no lung tumors were observed in 16 dogs with the lowest lung doses (8 to 22 cGy, mean 14.4 ± 7.6 c

  12. Historical reconstruction of Plutonium contamination in the Swiss-Italian Alps

    Directory of Open Access Journals (Sweden)

    Gabrieli J.

    2013-04-01

    Full Text Available Plutonium is present in the environment as a consequence of atmospheric nuclear tests carried out in the 1960s, nuclear weapons production and releases by the nuclear industry over the past 50 years. Approximately 6 tons of 239Pu have been released into the environment as a result of 541 atmospheric weapon tests Nuclear Pu fallout has been studied in various environmental archives, such as sediments, soil and herbarium grass. Mid-latitude ice cores have been studied as well, on Mont Blanc, the Western Alps and on Belukha Glacier, Siberian Altai. We present a Pu record obtained by analyzing 52 discrete samples of an alpine firn/ice core from Colle Gnifetti (M. Rosa, 4450 m a.s.l., dating from 1945 to 1991. The 239Pu signal was recorded directly, without preliminary cleaning or preconcentration steps, using an high resolution inductively plasma mass spectrometer equipped with a desolvation system. The 239Pu profile reflects the three main periods of atmospheric nuclear weapons testing: the earliest peak lasted from 1954/55 to 1958 and was caused by the first testing period reaching a maximum in 1958. Despite a temporary halt of testing in 1959/60, the Pu concentration decreased only by half with respect to the 1958 peak due to long atmospheric residence times. In 1961/62 Pu concentrations rapidly increased reaching a maximum in 1963. After the signing of the “Limited Test Ban Treaty” between USA and USSR in 1964, Pu deposition decreased very sharply reaching a minimum in 1967. The third period (1967-1975 is characterized by irregular Pu concentrations with smaller peaks which might be related to the deposition of Saharan dust contaminated by the French nuclear tests of the 1960s.

  13. {sup 69}Ga NMR in Pu{sub 1-x}Ga{sub x} (x < 0.01) alloy

    Energy Technology Data Exchange (ETDEWEB)

    Piskunov, Yu. [Institute of Metal Physics, Ural Branch of Russian Academy of Sciences, Kovalevskaya Str. 18, 620041 Ekaterinburg (Russian Federation)], E-mail: piskunov@imp.uran.ru; Mikhalev, K. [Institute of Metal Physics, Ural Branch of Russian Academy of Sciences, Kovalevskaya Str. 18, 620041 Ekaterinburg (Russian Federation); Zuev, Yu. [Russian Federal Nuclear Center, Institute of Technical Physics, Snezhinsk (Russian Federation); Verkhovskii, S.; Arkhipov, V. [Institute of Metal Physics, Ural Branch of Russian Academy of Sciences, Kovalevskaya Str. 18, 620041 Ekaterinburg (Russian Federation); Svyatov, I.; Podgornova, I.; Shestakov, A. [Russian Federal Nuclear Center, Institute of Technical Physics, Snezhinsk (Russian Federation); Ogloblichev, V.; Pogudin, A.; Buzlukov, A. [Institute of Metal Physics, Ural Branch of Russian Academy of Sciences, Kovalevskaya Str. 18, 620041 Ekaterinburg (Russian Federation)

    2007-10-11

    {sup 69}Ga nuclear magnetic resonance (NMR) experiments have been carried out on the Pu{sub 0.995}Ga{sub 0.005} alloy at temperatures between 20 and 420 K at magnetic field of 9.4 T to study the local charge symmetry and magnetic behavior of the Pu atoms surrounding solute Ga. In accordance with optical metallography and X-ray diffraction studies the investigated plates of alloy (20 mm x 3 mm x 0.2 mm) represent at room temperature the single {alpha}-phase material without any detectable macroscopic segregation of other phases (the corresponding volume fraction <0.03). It was revealed that the magnetic shift of the {sup 69}Ga NMR central line and the electric quadrupole broadening of the Ga NMR spectrum trace temperature dependence of the NMR parameters is observed for the {delta}-phase plutonium alloy Pu{sub 0.95}Ga{sub 0.05}. On the basis of {sup 69}Ga NMR and X-ray data obtained, it is suggested that specific microscopic areas with a size less than 100 nm exist in the {alpha}-phase plutonium alloys Pu{sub 0.995}Ga{sub 0.005}. The local charge and magnetic environment of the solute Ga in these microscopic areas are similar to the observed in the stabilized {delta}-Pu alloy.

  14. Study on reduction and back extraction of Pu(IV) by urea derivatives in nitric acid conditions

    Energy Technology Data Exchange (ETDEWEB)

    Ye, G.A.; Xiao, S.T.; Yan, T.H.; Lin, R.S.; Zhu, Z.W. [China Institute of Atomic Energy, P.O.Box 275(26), Beijing 102413 (China)

    2013-07-01

    The reduction kinetics of Pu(IV) by hydroxyl-semicarbazide (HSC), hydroxyurea (HU) and di-hydroxyurea (DHU) in nitric acid solutions were investigated separately with adequate kinetic equations. In addition, counter-current cascade experiments were conducted for Pu split from U in nitric acid media using three kinds of reductant, respectively. The results show that urea derivatives as a kind of novel salt-free reductant can reduce Pu(IV) to Pu(III) rapidly in the nitric acid solutions. The stripping experimental results showed that Pu(IV) in the organic phase can be stripped rapidly to the aqueous phase by the urea derivatives, and the separation factors of plutonium /uranium can reach more than 10{sup 4}. This indicates that urea derivatives is a kind of promising salt-free agent for uranium/plutonium separation. In addition, the complexing effect of HSC with Np(IV) was revealed, and Np(IV) can be back-extracted by HSC with a separation factor of about 20.

  15. Development of a Self-Consistent Model of Plutonium Sorption: Quantification of Sorption Enthalpy and Ligand-Promoted Dissolution

    Energy Technology Data Exchange (ETDEWEB)

    Powell, Brian [Clemson Univ., SC (United States); Kaplan, Daniel I [Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL); Arai, Yuji [Univ. of Illinois, Urbana-Champaign, IL (United States); Becker, Udo [Univ. of Michigan, Ann Arbor, MI (United States); Ewing, Rod [Stanford Univ., CA (United States)

    2016-12-29

    This university lead SBR project is a collaboration lead by Dr. Brian Powell (Clemson University) with co-principal investigators Dan Kaplan (Savannah River National Laboratory), Yuji Arai (presently at the University of Illinois), Udo Becker (U of Michigan) and Rod Ewing (presently at Stanford University). Hypothesis: The underlying hypothesis of this work is that strong interactions of plutonium with mineral surfaces are due to formation of inner sphere complexes with a limited number of high-energy surface sites, which results in sorption hysteresis where Pu(IV) is the predominant sorbed oxidation state. The energetic favorability of the Pu(IV) surface complex is strongly influenced by positive sorption entropies, which are mechanistically driven by displacement of solvating water molecules from the actinide and mineral surface during sorption. Objectives: The overarching objective of this work is to examine Pu(IV) and Pu(V) sorption to pure metal (oxyhydr)oxide minerals and sediments using variable temperature batch sorption, X-ray absorption spectroscopy, electron microscopy, and quantum-mechanical and empirical-potential calculations. The data will be compiled into a self-consistent surface complexation model. The novelty of this effort lies largely in the manner the information from these measurements and calculations will be combined into a model that will be used to evaluate the thermodynamics of plutonium sorption reactions as well as predict sorption of plutonium to sediments from DOE sites using a component additivity approach.

  16. Atmospheric deposition, resuspension, and root uptake of Pu in corn and other grain-producing agroecosystems near a nuclear fuel facility

    Energy Technology Data Exchange (ETDEWEB)

    Pinder, J.E. III; McLeod, K.W.; Adriano, D.C.; Corey, J.C.; Boni, A.L. (Savannah River Ecology Laboratory, Aiken, SC (USA))

    1990-12-01

    Plutonium released to the environment may contribute to dose to humans through inhalation or ingestion of contaminated foodstuffs. Plutonium contamination of agricultural plants may result from interception and retention of atmospheric deposition, resuspension of Pu-bearing soil particles to plant surfaces, and root uptake. Plutonium on vegetation surfaces may be transferred to grain surfaces during mechanical harvesting. Data obtained from corn grown near the U.S. Department of Energy's H-Area nuclear fuel chemical separations facility on the Savannah River Site were used to estimate parameters of a simple model of Pu transport in agroecosystems. The parameter estimates for corn were compared to those previously obtained for wheat and soybeans. Despite some differences in parameter estimates among crops, the relative importances of atmospheric deposition, resuspension, and root uptake were similar among crops. For even small deposition rates, the relative importances of processes for Pu contamination of corn grain should be: transfer of atmospheric depositi